Preparation method and application of iron and potassium co-doped carbon nitride ozone catalyst

By using iron-potassium co-doped carbon nitride catalyst, the problem of limited active sites in traditional carbon nitride catalysts has been solved, achieving highly efficient removal of pollutants from water with high removal rate and environmentally friendly characteristics.

CN118847185BActive Publication Date: 2026-08-25CHINESE RES ACAD OF ENVIRONMENTAL SCI
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Patent Information

Application Number
CN202411141309.2
Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
Filing Date
2024-08-20
Publication Date
2026-08-25
Estimated Expiration
2044-08-20

AI Technical Summary

Technical Problem

Traditional carbon nitride ozone catalysts have few active sites and low catalytic activity, making them difficult to effectively remove new pollutants from water.

Method used

A method for preparing iron-potassium co-doped carbon nitride catalysts was adopted. By doping with Fe and K, the physicochemical properties of the carbon substrate surface were regulated, new active sites were constructed, and ozone catalytic activity was enhanced.

Benefits of technology

It achieves efficient removal of pollutants such as ibuprofen, ketoprofen, DEET, or atrazine from water, and features high removal rate, mild reaction conditions, green and environmentally friendly operation, simple process, and easy recycling and regeneration of catalyst materials.

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Abstract

The present disclosure provides a preparation method and application of an iron-potassium co-doped carbon nitride ozone catalyst, which comprises the following steps: S1, adding urea, a potassium source and an iron source into pure water, heating and stirring, grinding after water evaporation, and obtaining an iron-potassium co-doped carbon nitride precursor; S2, placing the precursor in a muffle furnace for calcination treatment, and obtaining a reacted sample; and S3, cooling, purifying, drying and grinding the reacted sample, and obtaining the iron-potassium co-doped carbon nitride ozone catalyst. The iron-potassium co-doped carbon nitride ozone catalyst has excellent catalytic performance, strong universality, mild reaction conditions and a simple process flow, and can be used in the field of water pollution control.
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Description

Technical Field

[0001] This disclosure relates to the field of water pollution control technology, specifically to a method for preparing and applying an iron-potassium co-doped carbon nitride ozone catalyst. Background Technology

[0002] Water scarcity has become a major obstacle to sustainable economic and social development, and municipal wastewater reuse is an important way to solve this problem. Water quality safety is a crucial prerequisite for the use of reclaimed water in my country. Currently, new pollutants are frequently detected in various types of water, posing potential risks to human health and the ecological environment. Therefore, developing efficient technologies for treating new pollutants is of great significance.

[0003] Ozone catalytic oxidation technology, as a green and efficient water treatment technology, boasts advantages such as strong catalytic ability, high reactive oxygen production, and stability, showing great promise in the sustainable degradation of new environmental pollutants. The key to ozone catalytic oxidation technology is the selection of a highly efficient and stable ozone catalyst. Carbon nitride, as a common carbon material, has advantages such as simple synthesis, tunable electronic structure, and abundant raw materials, and has been successfully applied in the field of ozone catalysis. However, it inherently suffers from a limited number of active sites and low catalytic activity. Summary of the Invention

[0004] (a) Technical problems to be solved

[0005] In view of this, this disclosure provides a method for preparing and applying an iron-potassium co-doped carbon nitride ozone catalyst to solve the technical problems of traditional ozone catalysts, such as few active sites and low catalytic activity.

[0006] (II) Technical Solution

[0007] The first aspect of this disclosure provides a method for preparing an iron-potassium co-doped carbon nitride ozone catalyst, comprising: S1, adding urea, potassium source and iron source to pure water, heating and stirring, evaporating the water and grinding to obtain an iron-potassium co-doped carbon nitride precursor; S2, placing the precursor in a muffle furnace for calcination to obtain a reacted sample; S3, cooling, purifying, drying and grinding the reacted sample to obtain the iron-potassium co-doped carbon nitride ozone catalyst.

[0008] According to an embodiment of this disclosure, the molar ratio of urea, potassium source and iron source in S1 is (600~700):(1~12):1.

[0009] According to embodiments of this disclosure, the potassium source in S1 is selected from one or more of potassium chloride, potassium hydroxide, potassium sulfate, and potassium acetate.

[0010] According to embodiments of this disclosure, the iron source in S1 is selected from one or more of ferric chloride hexahydrate, ferric nitrate nonahydrate, and ferric sulfate pentahydrate.

[0011] According to an embodiment of this disclosure, the calcination temperature in S2 is 450~550 °C; the calcination time is 2~4 h.

[0012] According to an embodiment of this disclosure, the purification step in S3 includes filtration of the cooled sample and washing the precipitate obtained after filtration with deionized water and anhydrous ethanol, respectively.

[0013] According to an embodiment of this disclosure, the temperature of the drying step in S3 is 60~80 °C, and the time is 6~8 h.

[0014] The second aspect of this disclosure provides an iron-potassium co-doped carbon nitride ozone catalyst, which is prepared according to the aforementioned preparation method of the iron-potassium co-doped carbon nitride ozone catalyst.

[0015] The third aspect of this disclosure provides the use of the aforementioned iron-potassium co-doped carbon nitride ozone catalyst as an ozone catalyst for removing at least one of ibuprofen, ketoprofen, DEET, and atrazine from water.

[0016] The fourth aspect of this disclosure provides a method for removing ibuprofen, ketoprofen, DEET, or atrazine from water using an ozone catalyst, comprising: adding an ozone catalyst to an aqueous solution containing ibuprofen, ketoprofen, DEET, or atrazine, and stirring at room temperature; wherein the ozone catalyst is the aforementioned iron-potassium co-doped carbon nitride ozone catalyst; and introducing a certain concentration of ozone into the aqueous solution containing the ozone catalyst to degrade ibuprofen, ketoprofen, DEET, or atrazine.

[0017] (III) Beneficial Effects

[0018] This disclosure presents a method for preparing and applying an iron-potassium co-doped carbon nitride ozone catalyst. It provides a transition metal and alkali metal co-doping method that modifies the physicochemical properties of carbon nitride. Iron and potassium doping exhibit a synergistic effect: iron doping increases active sites, while potassium doping generates cyano groups, promoting the formation of nitrogen vacancies. Specifically, on one hand, nitrogen vacancies increase the local charge density on the catalyst surface, enhancing ozone adsorption and activation; on the other hand, potassium doping retains oxygen atoms in urea, allowing them to be captured by iron. This enables the iron oxide and carbon nitride to be linked through CO-Fe bonds, effectively promoting Fe... 2+Regeneration endows the catalyst with continuous degradation capabilities; the synergistic effect of metals and alkali metals accelerates ozone decomposition and the generation of reactive oxygen species, achieving higher catalytic activity. Furthermore, using iron-potassium co-doped carbon nitride materials as ozone catalysts to remove ibuprofen, ketoprofen, DEET, or atrazine from water offers advantages such as high removal rates, mild reaction conditions, simple process flow, environmental friendliness, energy saving, and simple and feasible preparation methods for the catalytic materials, as well as easy recycling and regeneration. Attached Figure Description

[0019] The above and other objects, features, and advantages of this disclosure will become clearer from the following description of embodiments of the present disclosure with reference to the accompanying drawings, in which:

[0020] Figure 1 A flowchart illustrating a method for preparing an iron-potassium co-doped carbon nitride ozone catalyst according to an embodiment of this disclosure is shown schematically.

[0021] Figure 2 A scanning electron microscope image of an iron-potassium co-doped carbon nitride ozone catalyst prepared according to embodiments of the present disclosure is shown schematically.

[0022] Figure 3 The schematic diagram shows the X-ray diffraction patterns of carbon nitride, iron-doped carbon nitride, potassium-doped carbon nitride, and iron-potassium co-doped carbon nitride ozone catalysts according to embodiments of the present disclosure;

[0023] Figure 4 This illustration schematically shows the effect of carbon nitride, iron-doped carbon nitride, potassium-doped carbon nitride, and iron-potassium co-doped carbon nitride ozone catalysts catalyzing the ozonation degradation of ibuprofen according to embodiments of this disclosure;

[0024] Figure 5 This illustration schematically shows the effect of iron-potassium co-doped carbon nitride ozone catalyst on the ozonation degradation of ibuprofen at different calcination temperatures according to embodiments of this disclosure;

[0025] Figure 6 The illustration shows the effect of iron-potassium co-doped carbon nitride ozone catalyst on the degradation of ketoprofen, DEET and atrazine by ozone according to embodiments of the present disclosure. Detailed Implementation

[0026] To make the objectives, technical solutions, and advantages of this disclosure clearer, the following detailed description is provided in conjunction with specific embodiments and the accompanying drawings.

[0027] The terminology used herein is for the purpose of describing particular embodiments only and is not intended to limit this disclosure. The terms “comprising,” “including,” etc., as used herein indicate the presence of the stated features, steps, operations, and / or components, but do not exclude the presence or addition of one or more other features, steps, operations, or components.

[0028] This disclosure aims to construct new active sites by regulating the physicochemical properties of carbon substrate surfaces, prepare environmental catalytic materials with high catalytic activity, construct a catalytic ozone oxidation system, and achieve efficient removal of recalcitrant pollutants from water bodies.

[0029] Based on this, this disclosure provides a method for preparing an iron-potassium co-doped carbon nitride ozone catalyst. Please refer to [link to relevant documentation]. Figure 1 The process includes: S1, adding urea, potassium source and iron source to pure water, heating and stirring, evaporating the water and grinding to obtain iron-potassium co-doped carbon nitride precursor; S2, placing the precursor in a muffle furnace for calcination to obtain the reacted sample; S3, cooling, purifying, drying and grinding the reacted sample to obtain iron-potassium co-doped carbon nitride ozone catalyst.

[0030] Specifically, S1 involves adding urea, potassium source, and iron source to pure water, heating and stirring in a constant-temperature magnetic stirrer at 60-80°C. After the water evaporates, the remaining solid is thoroughly ground in a mortar to obtain an iron-potassium co-doped carbon nitride precursor. The magnetic stirring in S1 ensures uniform mixing of the components in the solvent. S2 involves calcining the precursor in a muffle furnace under an air atmosphere, obtaining a solid sample after complete reaction. S3 involves cooling, purifying, drying, and grinding the reacted sample to obtain the iron-potassium co-doped carbon nitride material (Fe-K-CN).

[0031] The material preparation method disclosed herein is simple and feasible. Doping with Fe ions can provide new active sites, while the introduction of potassium ions promotes the generation of nitrogen vacancies, enhances the local charge density, promotes O3 activation, and enables Fe... 2+ / Fe 3+ The reversible cycle. The synergistic effect of transition metals and alkali metals accelerates ozone decomposition and the generation of reactive oxygen species, achieving higher catalytic activity.

[0032] Based on the above embodiments, the molar ratio of urea, potassium source and iron source in S1 is (600~700):(1~12):1.

[0033] When the molar ratio of urea, potassium source, and iron source is within the above range, it is beneficial to the synthesis of nitrogen defects on carbon nitride, thus giving the ozone catalyst better catalytic performance.

[0034] Based on the above embodiments, the potassium source in S1 is selected from one or more of potassium chloride, potassium hydroxide, potassium sulfate, and potassium acetate.

[0035] The reaction system can be acidic, neutral, or alkaline, and it exhibits good catalytic effects at pH 4 to 9, demonstrating the advantage of a wide pH range. The potassium source mentioned above also has the advantages of low price and readily available raw materials.

[0036] Based on the above embodiments, the iron source in S1 is selected from one or more of ferric chloride hexahydrate, ferric nitrate nonahydrate, and ferric sulfate pentahydrate.

[0037] Choosing one of the above-mentioned iron sources is beneficial for the thorough mixing of the iron source, urea, and potassium chloride, thereby achieving uniform dispersion and doping of metallic iron.

[0038] Based on the above embodiments, the calcination temperature in S2 is 450~550 ℃; the calcination time is 2~4 h.

[0039] The temperature and time of the muffle furnace calcination treatment are within the above range, which helps carbon nitride to be fully calcined under the action of potassium ions. On the other hand, it effectively combines with iron ions to form iron-potassium co-doped carbon nitride materials with good catalytic performance.

[0040] Based on the above embodiments, the purification step in S3 includes filtration of the cooled sample and washing the precipitate obtained after filtration with deionized water and anhydrous ethanol, respectively.

[0041] After the crucible cools, the reacted sample is removed, ground in a mortar, and then filtered using a vacuum filtration apparatus. The sample can be washed three times with deionized water and three times with anhydrous ethanol to better remove impurities.

[0042] Based on the above embodiments, the temperature of the drying step in S3 is 60~80 ℃ and the time is 6~8 h.

[0043] At the above-mentioned drying temperature and drying time, it is beneficial to remove the solvent in the material, and finally obtain a brown solid, namely Fe-K-CN.

[0044] This disclosure also provides an iron-potassium co-doped carbon nitride ozone catalyst, which is prepared according to the aforementioned preparation method of the iron-potassium co-doped carbon nitride ozone catalyst.

[0045] In this iron-potassium co-doped carbon nitride ozone catalyst, iron and potassium exhibit a synergistic effect. Iron doping increases the number of active sites, while potassium doping promotes the formation of nitrogen vacancies. On one hand, nitrogen vacancies increase the local charge density on the catalyst surface, enhancing ozone adsorption and activation; on the other hand, they promote the formation of Fe... 2+Effective regeneration endows the catalyst with continuous degradation capability, thereby improving the catalytic degradation efficiency of ozone. This iron-potassium co-doped carbon nitride ozone catalyst has advantages such as low cost and high efficiency as an ozone catalyst, and its preparation method is simple and easy to operate.

[0046] This disclosure also provides the use of the aforementioned iron-potassium co-doped carbon nitride ozone catalyst as an ozone catalyst for removing at least one of ibuprofen, ketoprofen, DEET, and atrazine from water.

[0047] In an ozone environment, the iron-potassium co-doped carbon nitride ozone catalyst generates more hydroxyl radicals and superoxide radicals through catalysis of ozone. These radicals react with pollutants in water, such as ibuprofen, ketoprofen, DEET, or atrazine, through reactions such as hydroxylation, ketation, decarboxylation, demethylation, side-chain decarboxylation, and aryl epoxidation, thereby achieving effective degradation of pollutants.

[0048] This disclosure also provides a method for removing ibuprofen, ketoprofen, DEET, or atrazine from water using an ozone catalyst, comprising: adding an ozone catalyst to an aqueous solution containing ibuprofen, ketoprofen, DEET, or atrazine, and stirring at room temperature; wherein the ozone catalyst is the aforementioned iron-potassium co-doped carbon nitride ozone catalyst; and introducing a certain concentration of ozone into the aqueous solution containing the ozone catalyst to degrade ibuprofen, ketoprofen, DEET, or atrazine.

[0049] Specifically, the method includes preparing an iron-potassium co-doped carbon nitride catalyst; introducing ozone at a dose of 0.05–0.35 g / L into water containing ibuprofen, ketoprofen, DEET, or atrazine pollutants; then adding an iron-potassium co-doped carbon nitride catalyst at a dose of 0.02–0.2 g / L; and reacting for 15–30 min, after which ibuprofen, ketoprofen, DEET, or atrazine are degraded.

[0050] The present disclosure will be further described below through specific embodiments. The following examples specifically illustrate the above-mentioned iron-potassium co-doped carbon nitride ozone catalyst, its preparation method, and its application. However, the following examples are merely illustrative of the present disclosure, and the scope of the disclosure is not limited thereto.

[0051] Example 1:

[0052] In this embodiment, the preparation method of an iron-potassium co-doped carbon nitride ozone catalyst is completed according to the following steps:

[0053] Step 1, Preparation of Fe-K-CN materials

[0054] (1) Add 0.1 g potassium chloride, 0.1 g ferric chloride hexahydrate and 15 g urea to 60 mL of pure water respectively, stir thoroughly at 60 °C for 180 min on a constant temperature magnetic stirrer, evaporate the water and grind thoroughly in a mortar to obtain iron potassium co-doped carbon nitride precursor.

[0055] (2) The iron-potassium co-doped carbon nitride precursor in (1) was placed in a muffle furnace and calcined at 550°C for 4 h under an air protective atmosphere, with a heating rate of 5 °C / min, to obtain the sample after reaction.

[0056] (3) The sample obtained in step (2) after reaction was filtered by a solvent filter and the precipitate obtained by filtration was washed three times each with deionized water and anhydrous ethanol. Then it was dried at 80 °C for 8 h and ground to obtain a brown solid, which is Fe-K-CN.

[0057] Step 2, Characterization of Fe-K-CN materials

[0058] Figure 2 This is a scanning electron microscope image of the Fe-K-CN catalyst prepared in Example 1 of this disclosure. The image shows that Fe2O3 and Fe3O4 nanoparticles were successfully combined with the sheet-like CN.

[0059] Figure 3 X-ray diffraction patterns of CN, Fe-CN, K-CN, and the Fe-K-CN composite catalyst prepared in Example 1 of this disclosure are shown. The characteristic diffraction peaks of the Fe-K-CN sample correspond to standard Fe2O3 (PDF 79-1741) and Fe3O4 (PDF 88-0315), respectively, and the diffraction peaks are clear and strong. No impurity peaks were observed, indicating that it has high crystallinity and high purity. The characteristic peaks of Fe-CN and Fe-K-CN are largely consistent. The characteristic peaks of the K-CN sample are largely consistent with those of CN, indicating that K-CN retains the original CN structure.

[0060] Step 3: Add Fe-K-CN and ozone to the mixed solution.

[0061] 0.1 g / L Fe-K-CN was added to water containing 10 mg / L ibuprofen and mixed. A certain concentration of ozone was added to the water, and the reaction was carried out at room temperature and under magnetic stirring for 15 min.

[0062] After treatment, the water quality was tested, and ibuprofen was found to have completely degraded.

[0063] Figure 4This diagram illustrates the degradation effect of ozone on ibuprofen using CN, Fe-CN, K-CN, and Fe-K-CN prepared according to the embodiments of this disclosure. As can be seen from the diagram, the Fe-K-CN catalyst prepared in Example 1 of this disclosure exhibits a more significant degradation effect under ozone conditions compared to other catalysts.

[0064] Example 2 (Calming temperature of Fe-K-CN preparation varied):

[0065] In this embodiment, a method for preparing an iron-potassium co-doped carbon nitride material is carried out according to the following steps:

[0066] Step 1, Preparation of Fe-K-CN materials

[0067] (1) Add 0.1 g potassium chloride, 0.1 g ferric chloride hexahydrate and 15 g urea to 60 mL of pure water respectively, stir thoroughly at 60 °C for 180 min on a constant temperature magnetic stirrer, evaporate the water and grind thoroughly in a mortar to obtain iron potassium co-doped carbon nitride precursor.

[0068] (2) The iron-potassium co-doped carbon nitride precursor in (1) was placed in a muffle furnace and calcined at 450, 500 and 550 °C respectively at a heating rate of 5 °C / min under the protective atmosphere of air for 4 h to obtain the sample after reaction.

[0069] (3) The sample obtained in step (2) after reaction was filtered by solvent filter and the precipitate obtained by filtration was washed three times each with deionized water and anhydrous ethanol. Then it was dried at 80 °C for 8 h and ground to obtain brown solids, namely Fe-K-CN-450, Fe-K-CN-500 and Fe-K-CN-550.

[0070] Step 3: Add Fe-K-CN and ozone to the mixed solution.

[0071] Add 0.1 g / L Fe-K-CN to water containing 10 mg / L ibuprofen, ketoprofen, DEET, or atrazine, add a certain concentration of ozone to the water, and react at room temperature with magnetic stirring for 15 minutes.

[0072] After treatment, water quality was tested, and ibuprofen, ketoprofen, DEET, or atrazine were found to have largely degraded.

[0073] Figure 5This diagram illustrates the degradation effect of ozone on ibuprofen catalyzed by Fe-K-CN-450, Fe-K-CN-500, and Fe-K-CN-550 prepared according to the embodiments of this disclosure. As can be seen from the diagram, the Fe-K-CN catalyst prepared by calcination at 550 °C in this disclosure exhibits a more significant degradation effect under ozone irradiation, achieving a degradation of over 50% of ibuprofen within 15 minutes. Figure 6 The diagram shows the degradation effect of Fe-K-CN catalyzed ozone on ketoprofen (KET), DEET, and atrazine (ATZ) prepared according to the embodiments of this disclosure. It can be seen that the Fe-K-CN catalyst has a good degradation effect on ketoprofen, DEET, or atrazine under the action of ozone.

[0074] Comparative Example 1 (using a single CN as a comparison):

[0075] In this embodiment, a method for preparing a carbon nitride material is carried out according to the following steps:

[0076] Step 1, Preparation of CN material

[0077] (1) Grind 15 g of urea and add it to the crucible to obtain carbon nitride precursor.

[0078] (2) The carbon nitride precursor described in (1) was placed in a muffle furnace and calcined at 550 °C for 4 h under an air protective atmosphere at a heating rate of 5 °C / min to obtain the sample after reaction.

[0079] (3) The sample obtained in step (2) after reaction was filtered by a solvent filter and the precipitate obtained by filtration was washed three times each with deionized water and anhydrous ethanol. The sample was then dried at 80 °C for 8 h to obtain a light yellow solid, which is CN.

[0080] Step 3: Add CN and ozone to the mixed solution.

[0081] 0.1 g / L CN was added to water containing 10 mg / L ibuprofen and mixed. A certain concentration of ozone was added to the water and the reaction was carried out at room temperature and under magnetic stirring for 15 min.

[0082] After treatment, water quality was tested, and ibuprofen was degraded by 62.60%.

[0083] Comparative Example 2 (using Fe-CN alone as a comparison):

[0084] (1) Add 0.1 g of ferric chloride hexahydrate and 15 g of urea to 60 mL of pure water, stir thoroughly at 60 °C for 180 min on a constant temperature magnetic stirrer, and after the water evaporates, grind thoroughly in a mortar to obtain iron-doped carbon nitride precursor.

[0085] (2) The iron-doped carbon nitride precursor described in (1) was placed in a muffle furnace and calcined at 550 °C for 4 h under an air protective atmosphere, with a heating rate of 5 °C / min, to obtain the sample after reaction.

[0086] (3) The sample obtained in step (2) after reaction was filtered by solvent filter, and the precipitate obtained by filtration was washed three times each with deionized water and anhydrous ethanol. Then it was dried at 80 °C for 8 h and ground to obtain a brown solid, which is Fe-CN.

[0087] Step 3: Add Fe-CN and ozone to the mixed solution.

[0088] 0.1 g / L Fe-CN was added to water containing 10 mg / L ibuprofen and mixed. A certain concentration of ozone was added to the water and the reaction was carried out at room temperature and under magnetic stirring for 15 min.

[0089] After treatment, water quality was tested, and ibuprofen was found to have degraded by 62.53%.

[0090] Comparative Example 3 (using K-CN alone as a comparison):

[0091] (1) Add 0.1 g potassium chloride and 15 g urea to 60 mL of pure water respectively, stir thoroughly at 60 °C for 180 min on a constant temperature magnetic stirrer, and after the water evaporates, grind thoroughly in a mortar to obtain potassium-doped carbon nitride precursor.

[0092] (2) The potassium-doped carbon nitride precursor described in (1) was placed in a muffle furnace and calcined at 550 °C for 4 h under an air protective atmosphere, with a heating rate of 5 °C / min, to obtain the sample after reaction.

[0093] (3) The sample obtained in step (2) after reaction was filtered by solvent filter, and the precipitate obtained by filtration was washed three times each with deionized water and anhydrous ethanol. Then it was dried at 80 °C for 8 h and ground to obtain a yellow solid, which is K-CN.

[0094] Step 3: Add K-CN and ozone to the mixed solution.

[0095] 0.1 g / L K-CN was added to water containing 10 mg / L ibuprofen and mixed. A certain concentration of ozone was added to the water and the reaction was carried out at room temperature and under magnetic stirring for 15 min.

[0096] After treatment, water quality was tested, and ibuprofen was found to have degraded by 78.91%.

[0097] Comparative Example 4 (without Fe-K-CN as a control):

[0098] In this embodiment, a method for preparing an iron-potassium co-doped carbon nitride material is carried out according to the following steps:

[0099] Step 1: Add ozone to the ibuprofen mixture.

[0100] A certain concentration of ozone was added to the water, and the reaction was carried out at room temperature and under magnetic stirring conditions for 15 minutes.

[0101] After treatment, water quality was tested, and ibuprofen was found to have degraded by 39.91%.

[0102] Comparative Example 5 (without O3 as a control):

[0103] In this embodiment, a method for preparing an iron-potassium co-doped carbon nitride material is carried out according to the following steps:

[0104] Step 1: Add Fe-K-CN to the ibuprofen mixed solution

[0105] 0.1 g of Fe-K-CN was added to the ibuprofen mixture, and the reaction was carried out at room temperature with magnetic stirring for 15 min.

[0106] After treatment, water quality was tested and found that ibuprofen did not degrade and Fe-K-CN had no adsorption effect.

[0107] In the iron-potassium co-doped carbon nitride ozone catalyst disclosed herein, iron and potassium have a synergistic effect. Potassium doping can promote the formation of nitrogen defects, effectively solving the problem that Fe catalytic sites are easily deactivated and the catalytic effect is poor in traditional iron-based carbon materials.

[0108] The specific embodiments described above further illustrate the purpose, technical solutions, and beneficial effects of this disclosure. It should be understood that the above descriptions are merely specific embodiments of this disclosure and are not intended to limit this disclosure. Any modifications, equivalent substitutions, improvements, etc., made within the spirit and principles of this disclosure should be included within the protection scope of this disclosure.

Claims

1. The use of a potassium-iron co-doped carbon nitride ozone catalyst as an ozone catalyst, wherein the ozone catalyst is used to remove at least one of ibuprofen, ketoprofen, DEET, and atrazine from water, and the method for preparing the potassium-iron co-doped carbon nitride ozone catalyst is characterized in that... include: S1, urea, potassium source and iron source are added to pure water, heated and stirred, the water is evaporated and then ground to obtain iron-potassium co-doped carbon nitride precursor, wherein the molar ratio of urea, potassium source and iron source is (600~700):(1~12):1; S2, the precursor is placed in a muffle furnace and calcined in air atmosphere to obtain the reacted sample, wherein the calcination temperature is 450~550 ℃ and the calcination time is 2~4 h; S3. The reacted sample is cooled, purified, dried, and ground to obtain an iron-potassium co-doped carbon nitride ozone catalyst.

2. The use according to claim 1, characterized in that, The potassium source mentioned in S1 is selected from one or more of potassium chloride, potassium hydroxide, potassium sulfate, and potassium acetate.

3. The use according to claim 1, characterized in that, The iron source mentioned in S1 is selected from one or more of ferric chloride hexahydrate, ferric nitrate nonahydrate, and ferric sulfate pentahydrate.

4. The use according to claim 1, characterized in that, The purification step described in S3 includes filtration of the cooled sample and washing the precipitate obtained after filtration with deionized water and anhydrous ethanol, respectively.

5. The use according to claim 1, characterized in that, The drying step described in S3 is performed at a temperature of 60-80 °C for 6-8 h.

6. The use according to claim 1, characterized in that, include: Add the ozone catalyst to an aqueous solution containing ibuprofen, ketoprofen, DEET, or atrazine, and stir at room temperature; A certain concentration of ozone is introduced into the aqueous solution containing the ozone catalyst to degrade the ibuprofen, ketoprofen, DEET, or atrazine.

Citation Information

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