A method for degrading paracetamol in water using a periodate activated with carbon-doped boron nitride
By activating periodate with a carbon-doped boron nitride catalyst, the secondary pollution problem caused by excessive addition of oxidants in the existing technology is solved, and the efficient degradation of acetaminophen is achieved, which is highly efficient and environmentally friendly.
Patent Information
- Application Number
- CN202311549625.9
- Authority / Receiving Office
- CN · China
- Patent Type
- Patents(China)
- Current Assignee / Owner
- Filing Date
- 2023-11-20
- Publication Date
- 2025-10-17
- Estimated Expiration
- 2043-11-20
AI Technical Summary
Existing non-metallic-based catalysts require the addition of excess oxidants during the activation of periodate to ensure efficient utilization, which leads to secondary pollution and reduced degradation efficiency. How to develop a catalyst with multiple surface active sites, high oxidant utilization efficiency, and environmental friendliness?
A carbon-doped boron nitride catalyst is prepared by polydopamine coating and high-temperature pyrolysis to enhance the activation effect on periodate and achieve efficient degradation of acetaminophen. The catalyst is made of boron nitride coated with polydopamine and calcined at high temperature to form carbon doping, which increases surface active sites and carbonyl groups and improves the utilization rate of the oxidant.
It achieves efficient degradation of acetaminophen with a degradation rate of 90.8%, high oxidant utilization rate, avoids secondary pollution caused by excessive oxidants, and has green and environmentally friendly characteristics.
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Figure CN117735696B_ABST
Abstract
Description
TECHNICAL FIELD
[0001] The present application belongs to the field of advanced oxidation treatment of environmental pollutants, and particularly relates to a method for degrading paracetamol in water by using carbon-doped boron nitride to activate periodic acid. BACKGROUND
[0002] Paracetamol is a commonly used antipyretic analgesic drug. Wastewater containing paracetamol and its partial degradation by-products can pose a threat to aquatic organisms and the ecological environment, and can also harm embryos, infants, children and physically weak adults as well as people sensitive to drugs. Therefore, it is crucial to develop a technology for effectively removing paracetamol.
[0003] The advanced oxidation process based on periodic acid (PI) has been widely used in the treatment of refractory organic pollutants due to its simple operation and strong oxidation ability. It is worth noting that due to the relatively low oxidation-reduction potential of PI (+1.6 eV), the ability of PI itself to oxidize organic pollutants is limited. Generally, ultraviolet light, ultrasound, sunlight, microwave, freezing, transition metal compounds (Co, Fe, Mn and Cu) can activate PI to produce active substances (IO3 • , ·OH, O2 •- , 1 O2 and O(3P) and the like), or degrade pollutants through non-radical pathways. However, high energy input, secondary pollution (inevitable metal leaching) and inherent defects of radical activation pathways (easily disturbed by water matrix in the environment background) limit their potential application in the above PI activation processes.
[0004] Boron nitride has a large specific surface area, high chemical stability and many structural defects, and has broad application prospects in water body remediation. Raw BN is considered to be an excellent co-catalyst for photodegradation, and modified boron nitride also has good activation effect on peroxide. However, in the process of activating periodic acid with non-metal-based catalysts, an excess of oxidizing agent is often added to ensure efficient utilization. Excessive oxidizing agent can lead to more serious secondary pollution, and even compete with pollutants and their by-products for free radicals, resulting in reduced degradation efficiency, which requires further improvement of the activation efficiency of modified boron nitride on periodic acid and the development of a low-dose oxidizing agent system. Therefore, how to obtain a boron nitride catalyst with high surface active site, high utilization efficiency of oxidizing agent and environmental friendliness is of great significance for efficient activation of periodic acid to degrade organic pollutants. SUMMARY
[0005] The technical problem solved by the present application is to overcome the shortcomings of the prior art and provide a method for degrading acetaminophen in water by using carbon-doped boron nitride to activate periodic acid, which has simple process, convenient operation, high treatment efficiency, small amount of oxidizing agent, good reusability and environmental friendliness.
[0006] To solve the above technical problems, the present application adopts the following technical solutions.
[0007] A method for degrading acetaminophen in water by using carbon-doped boron nitride to activate periodic acid, which is a method for degrading water containing acetaminophen by using carbon-doped boron nitride catalyst to activate periodic acid; the carbon-doped boron nitride catalyst is prepared by coating polydopamine on boron nitride and calcining, and the calcination temperature is 700-1000 DEG C.
[0008] The above method is further improved, and the preparation method of the carbon-doped boron nitride catalyst comprises the following steps:
[0009] S1, mixing boron nitride and tris-hydroxymethyl aminomethane buffer to obtain a suspension;
[0010] S2, adding dopamine hydrochloride to the suspension obtained in step S1, stirring, filtering, washing, drying to obtain polydopamine-coated boron nitride precursor;
[0011] S3, under the protection of inert gas, calcining the polydopamine-coated boron nitride precursor obtained in step S2 to obtain carbon-doped boron nitride catalyst.
[0012] The above method is further improved, and the calcination temperature is 800-1000 DEG C.
[0013] The above method is further improved, and the calcination temperature is 850-950 DEG C.
[0014] The above method is further improved, and the mass ratio of boron nitride to dopamine hydrochloride is 1-2:1-2.
[0015] The above method is further improved, and in step S1, the concentration of the tris-hydroxymethyl aminomethane buffer is 0.1-0.3 mol / L, the pH value of the tris-hydroxymethyl aminomethane buffer is 7-9, the mixing is carried out under stirring, and the stirring time is 30-90 min.
[0016] And / or, in step S2, the stirring temperature is 25 DEG C, the stirring time is 6-10 h, and after drying, the product is ground and sieved through a 100 mesh sieve.
[0017] And / or, in step S3, the calcination time is 1h-4h, the heating rate during the calcination process is 2℃ / min-5℃ / min, and the inert gas is argon.
[0018] The method is further improved, and the degradation treatment is that the carbon-doped boron nitride catalyst is mixed with the water body containing acetaminophen, stirred, and high iodate is added to perform a degradation reaction, so that the acetaminophen in the water body is degraded.
[0019] The method is further improved, and the ratio of the carbon-doped boron nitride catalyst to the water body containing acetaminophen is 0.05g-0.2g:1L, and the ratio of the high iodate to the water body containing acetaminophen is 30μmol-60μmol:1L.
[0020] The method is further improved, and the initial concentration of acetaminophen in the water body containing acetaminophen is 2.5mg / L-20mg / L, the initial pH value of the water body containing acetaminophen is 3-9, and the high iodate is metaperiodate sodium and / or orthoperiodate sodium.
[0021] The method is further improved, and the stirring time is 30min-60min, the degradation reaction time is 5min-10min, and the catalytic degradation reaction temperature is 10℃-50℃.
[0022] Compared with the prior art, the method has the following advantages:
[0023] In view of the defect that an excessive oxidant needs to be added in the existing non-metallic catalyst activation of high iodate process to ensure efficient utilization, the application creatively proposes a method for degrading acetaminophen in water by using carbon-doped boron nitride to activate high iodate, wherein the carbon-doped boron nitride catalyst used is prepared by simple polydopamine coating and high-temperature pyrolysis. The carbon-doped boron nitride catalyst of the application has a strong adhesion to various forms of surfaces due to the polydopamine, and a thin coating layer is formed on the surface of the boron nitride by polydopamine coating; then, the polydopamine-coated boron nitride precursor is pyrolyzed at high temperature to generate more carbonyl groups and defects, thereby enhancing the activation effect of the carbon-doped boron nitride catalyst on high iodate, and finally achieving efficient degradation of acetaminophen. In the application, the degradation rates of C-BN-700, C-BN-800, C-BN-900 and C-BN-1000 on acetaminophen within 8 minutes are 74.0%, 83.0%, 90.8% and 87.1% respectively; in particular, C-BN-900 exposes more active sites, so that it can better activate high iodate and achieve efficient utilization of high iodate, thereby enhancing the ability to degrade acetaminophen. The method of the application can efficiently activate low-dose high iodate oxidant by using the carbon-doped boron nitride catalyst, thereby efficiently degrading acetaminophen, and has the advantages of simple process, convenient operation, high oxidant utilization rate, fast degradation efficiency, good removal effect and the like, and is a green and environment-friendly method, which has practical significance for wastewater treatment in the environment. BRIEF DESCRIPTION OF DRAWINGS
[0024] Figure 1 SEM images of the carbon-doped boron nitride catalyst (C-BN-900) and the boron nitride catalyst (BN) prepared in Example 1 of the application.
[0025] Figure 2 TEM image of the carbon-doped boron nitride catalyst (C-BN-900) prepared in Example 1 of the application.
[0026] Figure 3 Elemental mapping of the carbon-doped boron nitride catalyst (C-BN-900) prepared in Example 1 of the application.
[0027] Figure 4 XRD patterns of the carbon-doped boron nitride catalyst (C-BN-700, C-BN-800, C-BN-900, C-BN-1000) and the boron nitride catalyst (BN) prepared in Example 1 of the application.
[0028] Figure 5 Raman spectra of the carbon-doped boron nitride catalyst (C-BN-700, C-BN-800, C-BN-900, C-BN-1000) prepared in Example 1 of the application.
[0029] Figure 6 XPS spectra of carbon-doped boron nitride catalysts (C-BN-700, C-BN-800, C-BN-900, C-BN-1000) prepared in Example 1 of the present application.
[0030] Figure 7 Degradation effect diagrams of carbon-doped boron nitride catalysts (C-BN-700, C-BN-800, C-BN-900, C-BN-1000) and boron nitride catalyst (BN) in activating periodate to degrade acetaminophen prepared in Example 1 of the present application.
[0031] Figure 8 Degradation effect diagrams of carbon-doped boron nitride catalysts in activating periodate to degrade acetaminophen prepared in Example 2 of the present application under different catalyst addition amounts.
[0032] Figure 9 Degradation effect diagrams of carbon-doped boron nitride catalysts in activating periodate to degrade acetaminophen prepared in Example 3 of the present application under different periodate addition amounts.
[0033] Figure 10 Degradation effect diagrams of carbon-doped boron nitride catalysts in activating periodate to degrade acetaminophen prepared in Example 4 of the present application under different pH conditions.
[0034] Figure 11 Degradation effect diagrams of carbon-doped boron nitride catalyst (C-BN-900) in degrading acetaminophen prepared in Example 5 of the present application under different temperature conditions. DETAILED DESCRIPTION
[0035] The present application will be further described in conjunction with the accompanying drawings and specific preferred embodiments, but the protection scope of the present application is not limited by the following embodiments. The materials and instruments used in the following embodiments are commercially available.
[0036] Example 1:
[0037] A method for degrading acetaminophen in water by using carbon-doped boron nitride to activate periodate, specifically, a method for degrading water containing acetaminophen by using carbon-doped boron nitride catalyst to activate periodate, comprising the following steps:
[0038] Take 10 mg of carbon-doped boron nitride catalyst (C-BN-700, C-BN-800, C-BN-900, C-BN-1000), boron nitride catalyst (BN), respectively, add 100 mL, 5 mg / L of acetaminophen solution (the initial pH of the solution is 5.8), use low-temperature circulating water device to keep the temperature at 25℃, stir for 30 min, reach adsorption-desorption equilibrium, then add sodium metaperiodate (chemical formula: NaIO4) (PI), so that the concentration of PI in the system is 40 μM, and carry out catalytic degradation reaction for 8 min to complete the degradation of acetaminophen in water.
[0039] During the catalytic degradation reaction, 1 mL of reaction solution was taken at 0 min (adsorption for 30 min), 1 min, 2 min, 3 min, 4 min, 5 min, 6 min, 7 min, 8 min, filtered with a 0.22 μm filter head, and added to a liquid phase vial pre-added with 100 μL of 100 mM sodium thiosulfate solution. The concentration of acetaminophen in the solution was detected by liquid chromatography.
[0040] PI group: no catalyst is added, and other conditions are the same.
[0041] C-BN-900 group: only C-BN-900 is added, PI is not added, and other conditions are the same.
[0042] In this embodiment, the carbon-doped boron nitride catalyst (C-BN-900) used is prepared by coating boron nitride with polydopamine and calcining, including the following steps:
[0043] (1) Take 0.5 g of boron nitride and add it to a pH = 8.5, 0.1 mol / L tris-hydroxymethyl aminomethane buffer solution, stir for 30 min to disperse, and make it uniformly suspended to obtain a suspension.
[0044] (2) Then add 0.5 g of dopamine hydrochloride to the above suspension, stir for 6 h at 25℃, filter, wash, dry, grind the dried product, and pass it through a 100 mesh sieve to obtain a polydopamine-coated boron nitride precursor.
[0045] In this step, dopamine hydrochloride can undergo self-polymerization and coating reaction on the surface of boron nitride under alkaline conditions.
[0046] (3) Put the above polydopamine-coated boron nitride precursor into a covered quartz boat and place it in a tube furnace. Under an argon atmosphere, heat it to 900℃ at a heating rate of 5℃ / min for 120 min. After natural cooling, take it out to obtain a carbon-doped boron nitride catalyst, which is named C-BN-900.
[0047] In this embodiment, carbon-doped boron nitride catalysts with different calcination temperatures were also prepared, and the preparation method was basically the same as that of the carbon-doped boron nitride catalyst (C-BN-900), except that the calcination temperature was 700 DEG C, 800 DEG C and 1000 DEG C, respectively. The prepared carbon-doped boron nitride catalysts were named C-BN-700, C-BN-800 and C-BN-1000, respectively.
[0048] In this embodiment, the preparation method of the boron nitride catalyst (BN) used includes the following steps:
[0049] 0.5 g of boron nitride was weighed into a covered quartz boat and placed in a tube furnace. The temperature was raised to 900 DEG C at a rate of 5 DEG C / min under an argon atmosphere and calcined for 120 min. After natural cooling, the boron nitride catalyst was taken out and named BN.
[0050] Figure 1 The SEM images of the carbon-doped boron nitride catalyst (C-BN-900) and the boron nitride catalyst (BN) prepared in Example 1 of the present application are shown in Figure 1 It can be seen from the SEM images that a layer of covering layer covers the surface of boron nitride, and the surface becomes rough. It is speculated that a layer of carbon is deposited on the surface of boron nitride after calcination of polydopamine (PDA).
[0051] Figure 2 The TEM images of the carbon-doped boron nitride catalyst (C-BN-900) prepared in Example 1 of the present application are shown in Figure 2 It can be seen from the TEM images that a layer of ultrathin layer is formed on the edge of boron nitride. In the enlarged HRTEM image, the lattice fringes are measured to be 0.35 nm, which corresponds well to the (002) crystal plane of boron nitride.
[0052] Figure 3 The element distribution maps of the carbon-doped boron nitride catalyst (C-BN-900) prepared in Example 1 of the present application are shown in Figure 3 It can be seen from the element distribution maps that B, C, N and O are uniformly distributed in the entire selected area, which indicates that carbon is encapsulated on boron nitride.
[0053] Figure 4 The XRD patterns of the carbon-doped boron nitride catalyst (C-BN-700, C-BN-800, C-BN-900 and C-BN-1000) and the boron nitride catalyst (BN) prepared in Example 1 of the present application are shown in Figure 4 It can be seen from the XRD patterns that after the peaks of the carbon-doped boron nitride catalyst are compared with the standard card, it is found that the characteristic peaks coincide with those of boron nitride, which indicates that the main phase composition of the carbon-doped boron nitride catalyst of the present application is boron nitride. In addition, with the increase of pyrolysis temperature, the diffraction peak intensity of (002) and (001) first decreases and then increases, which indicates that the pyrolysis treatment destroys the crystal lattice structure.
[0054] Figure 5 The Raman spectra of the carbon-doped boron nitride catalysts (C-BN-700, C-BN-800, C-BN-900, and C-BN-1000) prepared in Example 1 of the present invention are shown in FIG. Figure 5 It can be seen that with the increase of pyrolysis (calcination) temperature, I D / I G However, when the temperature rises to 1000℃, due to the breaking of chemical bonds and the reconstruction of graphitized network, I D / I G A slight decrease.
[0055] Figure 6 The XPS spectra of the carbon-doped boron nitride catalysts (C-BN-700, C-BN-800, C-BN-900, and C-BN-1000) prepared in Example 1 of the present invention are shown in FIG. Figure 6 The HR-XPS spectrum of C 1s can be decomposed into three peaks at 284.8 eV, 285.9 eV, and 288.6 eV, attributed to C-C, C-N, and C=O bonds, respectively. The carbonyl (C=O) content increases with increasing pyrolysis temperature, with C-BN-900 exhibiting the highest carbonyl content at 18.05%, followed by C-BN-1000 (17.02%), C-BN-800 (16.19%), and C-BN-700 (14.89%).
[0056] Figure 7 The figure shows the degradation effect of acetaminophen by activating periodate with the carbon-doped boron nitride catalysts (C-BN-700, C-BN-800, C-BN-900, C-BN-1000) and the boron nitride catalyst (BN) prepared in Example 1 of the present invention. Figure 7 As can be seen, the degradation rates of acetaminophen in both the BN / PI system and PI alone (PI group) were almost zero within 8 minutes. When C-BN-900 was used alone, it adsorbed 14.3% of the acetaminophen. In the C-BN-900 / PI system, C-BN-900 fully activated 40 μmol / L of PI, resulting in a degradation rate of 90.8% of acetaminophen within 8 minutes. This indicates that carbon doping increases the number of functional groups and defects on the catalyst surface, creating more electron transfer channels (as evidenced by electrochemical impedance spectroscopy). Furthermore, in the acetaminophen degradation system activated by carbon-doped boron nitride catalysts, the degradation efficiency ranked C-BN-900 > C-BN-1000 > C-BN-800 > C-BN-700, consistent with the variation in defect and carbonyl content of the carbon-doped boron nitride catalysts. Therefore, in terms of degradation efficiency, C-BN-900 was the catalyst prepared at the optimal pyrolysis temperature.
[0057] In summary, under the conditions of an initial pH of 5.8, a PI concentration of 40 μmol / L, and a catalyst dosage of 0.1 g / L, the C-BN-900 exhibits excellent catalytic performance and can degrade 90.8% of the acetaminophen within 8 min. It can be seen that the carbon-doped boron nitride catalyst (C-BN-900) of the present application can achieve efficient removal of acetaminophen. In addition, the present application uses a lower oxidant dosage, avoids the addition of excessive oxidant to reduce the utilization rate of the oxidant, and thereby causes the problem of secondary pollution.
[0058] Example 2
[0059] The effect of different catalyst dosages on the degradation of acetaminophen was investigated, and the carbon-doped boron nitride catalyst was used to activate the high iodate to degrade acetaminophen in water, including the following steps:
[0060] 5 mg, 10 mg, 15 mg, and 20 mg of the carbon-doped boron nitride catalyst (C-BN-900) in Example 1 were respectively weighed and added to 100 mL of a 5 mg / L acetaminophen solution (the initial pH of the solution was 5.8), a low-temperature circulating water device was used to keep the temperature at 25°C, stirring was performed for 30 min to reach adsorption-desorption equilibrium, then sodium periodate (PI) was added to make the PI concentration in the system 40 μM, and a catalytic degradation reaction was performed for 8 min to complete the degradation of acetaminophen in water.
[0061] Figure 8 The degradation effect diagram of the carbon-doped boron nitride catalyst activated high iodate degrading acetaminophen under different catalyst dosages in Example 2 of the present application. Figure 8 It can be known from the diagram that the dosage of the C-BN-900 catalyst has a significant positive effect on the degradation of acetaminophen.
[0062] Example 3
[0063] The effect of different high iodate dosages on the degradation of acetaminophen was investigated, and the carbon-doped boron nitride catalyst was used to activate the high iodate to degrade acetaminophen in water, including the following steps:
[0064] 4 portions of 10 mg of the carbon-doped boron nitride catalyst (C-BN-900) in Example 1 were weighed and added to 100 mL of a 5 mg / L acetaminophen solution (the initial pH of the solution was 5.8), a low-temperature circulating water device was used to keep the temperature at 25°C, stirring was performed for 30 min to reach adsorption-desorption equilibrium, then sodium periodate (PI) was added to make the PI concentration in the system 30 μM, 40 μM, 50 μM, and 60 μM, respectively, and a catalytic degradation reaction was performed for 8 min to complete the degradation of acetaminophen in water.
[0065] Figure 9 The degradation effect diagram of the degradation of acetaminophen by the carbon-doped boron nitride catalyst activated periodate in different periodate addition amounts in the embodiment 3 of the present application is shown in the following figure. Figure 9 It can be seen that when the amount of periodate is increased from 30 μmol / L to 60 μmol / L, the degradation efficiency of acetaminophen first increases and then remains unchanged, which may be attributed to the fact that the active sites on the surface of C-BN-900 cannot accommodate more periodate.
[0066] Embodiment 4:
[0067] The influence of different pH values on the degradation effect of acetaminophen was investigated, specifically, the degradation of acetaminophen in water by the carbon-doped boron nitride catalyst activated periodate, including the following steps:
[0068] Four portions of acetaminophen solution (the concentration of the solution is 5 mg / L, and the volume is 100 mL) were taken, and 0.1 mol / L hydrochloric acid and sodium hydroxide solution were used to adjust the pH of the four portions of acetaminophen solution to 3, 5, 7 and 9, respectively. 10 mg of carbon-doped boron nitride catalyst (C-BN-900) in embodiment 1 was added, a low-temperature circulating water device was used to keep the temperature at 25°C, and stirring was performed for 30 min to achieve adsorption-desorption equilibrium. Then, sodium periodate (PI) was added to make the concentration of PI in the system 40 μM, and the catalytic degradation reaction was performed for 8 min to complete the degradation of acetaminophen in water.
[0069] During the catalytic degradation reaction, 1 mL of reaction solution was taken at 0 min (adsorption for 30 min), 1 min, 2 min, 3 min, 4 min, 5 min, 6 min, 7 min and 8 min, filtered with a 0.22 μm filter head, and added to a liquid phase vial in which 100 μL of 100 mM sodium thiosulfate solution had been previously added. The concentration of acetaminophen in the solution was detected by liquid chromatography.
[0070] Figure 10 The degradation effect diagram of the degradation of acetaminophen by the carbon-doped boron nitride catalyst activated periodate in different pH conditions in the embodiment 4 of the present application is shown in the following figure. Figure 10 It can be seen that the removal rates of acetaminophen by C-BN-900 at pH values of 3, 5, 7 and 9 are 96.4%, 88.8%, 73.7% and 71.0%, respectively. C-BN-900 has the best degradation effect on acetaminophen at pH 3, which may be because: at a lower pH value, H + may react with free electrons to generate hydrogen atoms (H•), which is one of the main reducing substances in acidic solutions, and H• can further react with IO4- Reaction to generate IO3 • Due to the significant improvement of the degradation efficiency of acetaminophen under acidic conditions, it is shown that in the C-BN-900 / PI system, H•induced IO4 - The reduction reaction is reasonable and feasible. In addition, the degradation efficiency of acetaminophen is more than 70% in the range of this study, and it can be seen that the pH range of the degradation system constructed by the carbon-doped boron nitride catalyst and PI in the present application is wide. The reaction formula occurring in the catalytic degradation process is shown as formula (1) and (2).
[0071]
[0072] Example 5:
[0073] The effect of different temperatures on the degradation of acetaminophen was investigated, which was the degradation of acetaminophen in water by activating periodate with carbon-doped boron nitride catalyst, including the following steps:
[0074] 4 portions of 10 mg of carbon-doped boron nitride catalyst (C-BN-900) in Example 1 were weighed and added to 100 mL of 5 mg / L acetaminophen solution (the initial pH of the solution was 5.8), and a low-temperature circulating water device was used to maintain the temperature at 15℃, 25℃, 35℃ and 45℃, respectively, and stirred for 30 min to reach adsorption-desorption equilibrium, then sodium periodate (PI) was added to make the concentration of PI in the system 40 μM, and the catalytic degradation reaction was carried out for 8 min to complete the degradation of acetaminophen in water.
[0075] During the catalytic degradation reaction process, 1 mL of reaction solution was taken at 0 min (adsorption for 30 min), 1 min, 2 min, 3 min, 4 min, 5 min, 6 min, 7 min, 8 min, and filtered with a 0.22 μm filter head, and added to a liquid phase vial pre-added with 100 μL of 100 mM sodium thiosulfate solution, and the concentration of acetaminophen in the solution was detected by liquid chromatography.
[0076] Figure 11 The degradation effect of carbon-doped boron nitride catalyst (C-BN-900) in Example 5 on acetaminophen at different temperatures. From Figure 11 It can be seen that when the temperature increases from room temperature to 45℃, the degradation efficiency of acetaminophen only increases slightly, and when the temperature is 15℃, the degradation efficiency decreases from 90.8% to 85.8%, which shows that the temperature has no significant effect on the degradation efficiency of acetaminophen, which may be related to the stability of periodate.
[0077] In summary, the method for degrading acetaminophen in water by using carbon-doped boron nitride to activate periodic acid has the advantages of simple process, convenient operation, high treatment efficiency, small amount of oxidant, good reusability, environmental friendliness, etc., can realize efficient removal of acetaminophen in water, has high use value and good application prospect.
[0078] The above is only a preferred embodiment of the present application, and does not limit the present application in any form. Although the present application has been disclosed as above with a preferred embodiment, it is not intended to limit the present application. Any person skilled in the art can make many possible changes and modifications to the technical solutions of the present application, or modify equivalent embodiments, without departing from the spirit and technical solutions of the present application, by using the disclosed methods and technical contents. Therefore, any simple modification, equivalent replacement, equivalent change and modification of the above embodiments made according to the technical essence of the present application, without departing from the technical solutions of the present application, still belongs to the protection scope of the technical solutions of the present application.
Claims
1. A method for degrading acetaminophen in water by activating periodate using carbon-doped boron nitride, characterized in that: The method utilizes a carbon-doped boron nitride catalyst to activate periodate to degrade acetaminophen-containing water; the carbon-doped boron nitride catalyst is prepared by coating boron nitride with polydopamine and calcining the boron nitride; the calcination temperature is 700°C to 1000°C.
2. The method for degrading acetaminophen in water by activating periodate with carbon-doped boron nitride according to claim 1, characterized in that: The preparation method of the carbon-doped boron nitride catalyst comprises the following steps: S1, mixing boron nitride and tris (hydroxymethyl)aminomethane buffer to obtain a suspension; S2. Add dopamine hydrochloride to the suspension obtained in step S1, stir, filter, wash, and dry to obtain a polydopamine-coated boron nitride precursor; S3. Under the protection of an inert gas, calcining the polydopamine-coated boron nitride precursor obtained in step S2 to obtain a carbon-doped boron nitride catalyst.
3. The method for degrading acetaminophen in water by activating periodate with carbon-doped boron nitride according to claim 2, characterized in that: The calcination temperature is 800°C to 1000°C.
4. The method for degrading acetaminophen in water by activating periodate with carbon-doped boron nitride according to claim 3, characterized in that: The calcination temperature is 850°C to 950°C.
5. The method for degrading acetaminophen in water by activating periodate with carbon-doped boron nitride according to claim 4, characterized in that: The mass ratio of the boron nitride to dopamine hydrochloride is 1-2:1-2.
6. The method for degrading acetaminophen in water by activating periodate with carbon-doped boron nitride according to claim 5, characterized in that: In step S1, the concentration of the Tris buffer is 0.1 mol / L to 0.3 mol / L, the pH value of the Tris buffer is 7 to 9, the mixing is performed under stirring, and the stirring time is 30 min to 90 min; And / or, in step S2, the stirring temperature is 25° C., the stirring time is 6 h to 10 h, and after the drying, the following treatment is further included: grinding the dried product and passing it through a 100-mesh sieve; And / or, in step S3, the calcination time is 1 hour to 4 hours, the heating rate during the calcination process is 2°C / min to 5°C / min, and the inert gas is argon.
7. The method for degrading acetaminophen in water by activating periodate with carbon-doped boron nitride according to any one of claims 1 to 6, characterized in that: The degradation treatment comprises: mixing a carbon-doped boron nitride catalyst with water containing acetaminophen, stirring, and adding periodate to carry out a degradation reaction, thereby achieving degradation of acetaminophen in the water.
8. The method for degrading acetaminophen in water by activating periodate with carbon-doped boron nitride according to claim 7, characterized in that: The ratio of the carbon-doped boron nitride catalyst to the water containing acetaminophen is 0.05 g to 0.2 g:1 L, and the ratio of the periodate to the water containing acetaminophen is 30 μmol to 60 μmol:1 L.
9. The method for degrading acetaminophen in water by activating periodate with carbon-doped boron nitride according to claim 8, characterized in that: The initial concentration of paracetamol in the paracetamol-containing water body is 2.5 mg / L to 20 mg / L, the initial pH value of the paracetamol-containing water body is 3 to 9, and the periodate is sodium metaperiodate and / or sodium orthoperiodate.
10. The method for degrading acetaminophen in water by activating periodate using carbon-doped boron nitride according to claim 9, characterized in that: The stirring time before the degradation reaction is 30 min to 60 min, the degradation reaction time is 5 min to 10 min, and the degradation reaction temperature is 10° C. to 50° C.