CN117205956B - Simple preparation method and application of modified carbon nitride - Google Patents
Simple preparation method and application of modified carbon nitride Download PDFInfo
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- CN117205956B CN117205956B CN202311292768.6A CN202311292768A CN117205956B CN 117205956 B CN117205956 B CN 117205956B CN 202311292768 A CN202311292768 A CN 202311292768A CN 117205956 B CN117205956 B CN 117205956B
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Abstract
The invention relates to a simple preparation method of modified carbon nitride and application thereof, urea is put into a baking oven to obtain dry urea; placing the dried urea into a crucible with a cover for calcination to obtain original carbon nitride; and (3) placing the original carbon nitride into ultrapure water, applying xenon lamp illumination for a certain time, filtering and vacuum drying to obtain the modified carbon nitride. The invention also utilizes modified carbon nitride to catalyze and adsorb and decolor the high-concentration cationic dye wastewater. The modified carbon nitride obtained by the invention has better electrostatic adsorption performance than the traditional physical adsorption performance, and has the advantages of high photocatalysis efficiency, remarkable decoloring effect, simple process and no secondary pollution.
Description
Technical Field
The invention belongs to the technical field of printing and dyeing wastewater treatment, and particularly relates to a simple preparation method and application of modified carbon nitride (GCN).
Background
Printing and dyeing wastewater is one of industrial wastewater difficult to degrade, and dye in the wastewater can only be transferred from a water phase to a solid phase by using a traditional adsorption and chemical precipitation method and cannot be effectively degraded. Compared with the traditional physical, chemical and biological means, the photocatalysis technology has the advantages of simple operation, mild reaction condition, quick degradation, high efficiency, no secondary pollution and the like.
The g-C 3N4 photocatalyst still has better stability under the irradiation of light in a strong acid or alkali solution due to strong covalent bonds between carbon and nitrogen atoms, and is a material with great potential for treating dye wastewater by photocatalysis. However, the conventional bulk g-C 3N4 generally has the defects of small specific surface area, narrow visible light response range, high electron-hole recombination rate, low carrier transmission efficiency and the like, and severely limits the exposure of surface active sites and the application of the bulk g-C 3N4 in a liquid-phase catalytic reaction system.
Disclosure of Invention
The invention discloses a simple preparation method and application of modified carbon nitride (GCN) for solving the problem that the effect is not ideal when dye wastewater is treated by photocatalysis due to the defects of wide band gap, low visible light utilization rate, easiness in compounding photogenerated carriers and the like of the traditional g-C 3N4.
The invention provides the following technical scheme: a simple preparation method of modified carbon nitride (GCN) comprises the following steps:
S1, putting urea into a baking oven to obtain dry urea;
s2, placing the dried urea into a crucible with a cover for calcination to obtain porous nano flaky carbon nitride doped with oxygen;
s3, placing the original carbon nitride into ultrapure water, applying xenon lamp illumination for a certain time, and then filtering and vacuum drying to obtain the modified carbon nitride.
Further, the drying temperature of the oven in the step S1 is 105 ℃, and the drying time is 12h.
Further, in the step S2, the amount of the added dry urea is 30 g, the volume of a crucible used is 30 mL, and the outside is wrapped by tinfoil paper; the calcination temperature was 550 ℃, the calcination time was 1h, and the temperature rise rate was 2.5 ℃/min.
Further, in the step S3, the original carbon nitride is added in an amount of 0.1 g, the ultrapure water is 200 mL, and the illumination time is respectively 0.5-5 h; the drying temperature was 60℃and the time was 12h.
The invention also provides application of the modified carbon nitride (GCN) to photocatalytic adsorption decoloration of high-concentration dye wastewater, which comprises the following specific steps: a certain amount of photocatalyst is taken and put into a condensing beaker, and is evenly dispersed in a certain concentration volume of methylene blue water solution by ultrasound. Before photoreaction, the closed paper box is used for covering the solution to simulate a dark environment, continuous stirring is carried out, the adsorption and desorption balance is achieved, and a syringe is used for sucking samples and sequencing. Then the xenon lamp is turned on to illuminate, and the top of the beaker is covered by quartz glass to prevent the liquid from heating and volatilizing. During which time samples were taken with syringe and filter and ordered. After sampling, absorbance values of the methylene blue stock solution and the above samples were measured with an ultraviolet spectrophotometer.
Further, the amount of the added GCN photocatalyst is 0.2 g, the high-concentration dye wastewater is 50 mg/L methylene blue aqueous solution, and the volume is 200 mL.
Further, the dark reaction adsorption and desorption time is 30 min, the illumination time is 60 min, the interval sampling time is 10min, and the sampling volume is 3 mL each time.
Further, the methylene blue aqueous solution has an ultraviolet test wavelength of 664 nm.
Through the technical scheme, the invention has the beneficial effects that:
1. by placing the traditional carbon nitride into ultrapure water and applying light source illumination, the structure of the carbon nitride is changed, the hydroxyl-OH functional group is increased, and the modified carbon nitride (GCN) with negative charges on the surface is obtained; meanwhile, the band gap is reduced, the separation efficiency of the photogenerated carriers is greatly improved, and the defects of narrow visible light response range, high electron-hole recombination rate, low carrier transmission efficiency and the like of the traditional g-C 3N4 are effectively overcome.
2. Compared with the traditional physical, chemical and biological means, the method is very suitable for the adsorption and decoloration treatment of high-concentration cationic dye wastewater, uniformly mixes the photocatalyst and the dye wastewater, has obvious decoloration effect in very short time due to the electrostatic adsorption effect under the condition of visible light, and has the advantages of simple treatment process, mild reaction condition, quick degradation, high efficiency and no secondary pollution.
Drawings
FIG. 1 shows XPS spectra C1 s, N1 s and O1 s of GCN-0, GCN-2 and GCN-5.
FIG. 2 shows PL spectra of GCN-0, GCN-2 and GCN-5, and time resolved photoluminescence spectra.
FIG. 3 is a graph showing the photocatalytic methylene blue adsorption decoloring performance and the first order reaction kinetics fit of GCN synthesized under different ultrapure water illumination conditions.
FIG. 4 is a graph showing the synthesized GCN photocurrent spectrum under different ultra pure water illumination conditions.
Detailed Description
The following description of the technical solutions in the embodiments of the present invention will be clear and complete, and it is obvious that the described embodiments are only some embodiments of the present invention, but not all embodiments. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
A simple preparation method of modified carbon nitride (GCN) comprises the following steps:
S1, putting urea into a baking oven to obtain dry urea;
S2, placing the dried urea into a crucible with a cover for calcination to obtain original carbon nitride, wherein the original carbon nitride is porous nano sheet-shaped oxygen-doped carbon nitride;
s3, placing the original carbon nitride into ultrapure water, applying xenon lamp illumination for a certain time, and then filtering and vacuum drying to obtain the modified carbon nitride.
In one embodiment, the oven drying temperature is 105 ℃ and the drying time is 12 h;
In one embodiment, the amount of added dry urea is 30 g, the crucible volume used is 30 mL, and the exterior is covered with tinfoil.
In one embodiment, the calcination temperature is 550 ℃, the calcination time is 1 h ℃, and the temperature rise rate is 2.5 ℃/min, thus obtaining the original carbon nitride.
In one embodiment, the original carbon nitride is placed in ultrapure water and a xenon lamp is applied for a certain period of time, followed by filtration and vacuum drying to obtain the modified carbon nitride.
In one embodiment, the amount of added raw carbon nitride is 0.1g, ultrapure water is 200 mL, and the illumination time is 0.5, 1,2,3, 5 and h respectively; the drying temperature was 60℃and the time was 12 h.
In one embodiment, the method for photocatalytic adsorption decolorization of high-concentration dye wastewater comprises the following specific steps: a certain amount of photocatalyst is taken and put into a condensing beaker, and is evenly dispersed in a certain concentration volume of methylene blue water solution by ultrasound. Before photoreaction, the closed paper box is used for covering the solution to simulate a dark environment, continuous stirring is carried out, the adsorption and desorption balance is achieved, and a syringe is used for sucking samples and sequencing. Then the xenon lamp is turned on to illuminate, and the top of the beaker is covered by quartz glass to prevent the liquid from heating and volatilizing. During which time samples were taken with syringe and filter and ordered. After sampling, absorbance values of the methylene blue stock solution and the above samples were measured with an ultraviolet spectrophotometer.
In one example, the amount of modified carbon nitride added was 0.2 g, the high concentration dye waste water was 50 mg/L methylene blue aqueous solution, and the volume was 200 mL.
In one embodiment, the dark reaction adsorption and desorption time is 30 min, the illumination time is 60min, the interval sampling time is 10min, and the sampling volume is 3 mL each time.
In one embodiment, the methylene blue aqueous solution has an ultraviolet test wavelength of 664 nm.
Example 1
Weighing 30 g urea, adding into a beaker, putting into an oven, drying at 105 ℃ for 12: 12h, after drying, putting the dried urea into a 30mL clean ceramic crucible, completely wrapping with aluminum foil, covering two layers of the crucible with matched crucible covers, putting into a muffle furnace, heating at a heating rate of 2.5 ℃/min, and calcining at 550 ℃ for 1: 1 h. After the completion of calcination, the mixture was cooled to room temperature and then taken out, and the mixture was ground to obtain an original carbon nitride powder (GCN-0). Then, 0.1 g of the original carbon nitride powder was placed in 200mL ultra pure water, and xenon lamp light was applied for 0.5 h, followed by filtration and vacuum drying to obtain modified carbon nitride (GCN-0.5). Then 0.2 g modified carbon nitride was taken and placed in a condensing beaker and evenly dispersed in 200mL of 50 mg/L methylene blue aqueous solution by ultrasound. Before photoreaction, the solution is covered by a closed paper box to simulate a dark environment, the solution is continuously stirred for 30min to reach adsorption and desorption equilibrium, and 3 mL samples are sucked by a syringe every 10min and are sequenced. Then the xenon lamp is turned on for illumination, and the illumination time is 60 min. During which 3 mL samples were aspirated every 10min a by syringe and ordered. After sampling, the absorbance of the methylene blue stock solution and the above sample was measured at 664 nm wavelength with an ultraviolet spectrophotometer.
Example 2
Weighing 30 g urea, adding into a beaker, putting into an oven, drying at 105 ℃ for 12: 12h, after drying, putting the dried urea into a 30 mL clean ceramic crucible, completely wrapping with aluminum foil, covering two layers of the crucible with matched crucible covers, putting into a muffle furnace, heating at a heating rate of 2.5 ℃/min, and calcining at 550 ℃ for 1:1 h. After the calcination, the mixture was cooled to room temperature and taken out, and the mixture was ground to obtain an original carbon nitride powder. Then, 0.1 g of the original carbon nitride was placed in 200 mL ultrapure water, and xenon lamp light 1 h was applied, followed by filtration and vacuum drying to obtain modified carbon nitride (GCN-1). Then 0.2 g modified carbon nitride was taken and placed in a condensing beaker and evenly dispersed in 200 mL of 50 mg/L methylene blue aqueous solution by ultrasound. Before photoreaction, the solution is covered by a closed paper box to simulate a dark environment, the solution is continuously stirred for 30 min to reach adsorption and desorption equilibrium, and 3 mL samples are sucked by a syringe every 10 min and are sequenced. Then the xenon lamp is turned on for illumination, and the illumination time is 60 min. During which 3 mL samples were aspirated every 10 min a by syringe and ordered. After sampling, the absorbance of the methylene blue stock solution and the above sample was measured at 664 nm wavelength with an ultraviolet spectrophotometer.
Example 3
Weighing 30 g urea, adding into a beaker, putting into an oven, drying at 105 ℃ for 12: 12 h, after drying, putting the dried urea into a30 mL clean ceramic crucible, completely wrapping with aluminum foil, covering two layers of the crucible with matched crucible covers, putting into a muffle furnace, heating at a heating rate of 2.5 ℃/min, and calcining at 550 ℃ for 1: 1 h. After the calcination, the mixture is cooled to room temperature and taken out, and the original carbon nitride is obtained by grinding. Then, 0.1 g of the original carbon nitride was placed in 200 mL ultrapure water, and xenon lamp light was applied for 2 h, followed by filtration and vacuum drying to obtain modified carbon nitride (GCN-2). Then 0.2 g modified carbon nitride was taken and placed in a condensing beaker and evenly dispersed in 200 mL of 50 mg/L methylene blue aqueous solution by ultrasound. Before photoreaction, the solution is covered by a closed paper box to simulate a dark environment, the solution is continuously stirred for 30 min to reach adsorption and desorption equilibrium, and 3 mL samples are sucked by a syringe every 10 min and are sequenced. Then the xenon lamp is turned on for illumination, and the illumination time is 60 min. During which 3 mL samples were aspirated every 10 min a by syringe and ordered. After sampling, the absorbance of the methylene blue stock solution and the above sample was measured at 664 nm wavelength with an ultraviolet spectrophotometer.
Example 4
Weighing 30 g urea, adding into a beaker, putting into an oven, drying at 105 ℃ for 12: 12h, after drying, putting the dried urea into a 30 mL clean ceramic crucible, completely wrapping with aluminum foil, covering two layers of the crucible with matched crucible covers, putting into a muffle furnace, heating at a heating rate of 2.5 ℃/min, and calcining at 550 ℃ for 1:1 h. After the calcination, the mixture was cooled to room temperature and taken out, and the mixture was ground to obtain an original carbon nitride powder. Then, 0.1 g of the original carbon nitride was placed in 200 mL ultrapure water, and xenon lamp light was applied for 3 h, followed by filtration and vacuum drying to obtain modified carbon nitride (GCN-3). Then 0.2 g modified carbon nitride was taken and placed in a condensing beaker and evenly dispersed in 200 mL of 50 mg/L methylene blue aqueous solution by ultrasound. Before photoreaction, the solution is covered by a closed paper box to simulate a dark environment, the solution is continuously stirred for 30 min to reach adsorption and desorption equilibrium, and 3 mL samples are sucked by a syringe every 10 min and are sequenced. Then the xenon lamp is turned on for illumination, and the illumination time is 60 min. During which 3 mL samples were aspirated every 10 min a by syringe and ordered. After sampling, the absorbance of the methylene blue stock solution and the above sample was measured at 664 nm wavelength with an ultraviolet spectrophotometer.
Example 5
Weighing 30 g urea, adding into a beaker, putting into an oven, drying at 105 ℃ for 12: 12h, after drying, putting the dried urea into a 30 mL clean ceramic crucible, completely wrapping with aluminum foil, covering two layers of the crucible with matched crucible covers, putting into a muffle furnace, heating at a heating rate of 2.5 ℃/min, and calcining at 550 ℃ for 1:1 h. After the calcination, the mixture was cooled to room temperature and taken out, and the mixture was ground to obtain an original carbon nitride powder. Then, 0.1 g of the original carbon nitride was placed in 200 mL ultrapure water, and xenon lamp light was applied for 5h, followed by filtration and vacuum drying to obtain modified carbon nitride (GCN-5). Then 0.2 g modified carbon nitride was taken and placed in a condensing beaker and evenly dispersed in 200 mL of 50 mg/L methylene blue aqueous solution by ultrasound. Before photoreaction, the solution is covered by a closed paper box to simulate a dark environment, the solution is continuously stirred for 30 min to reach adsorption and desorption equilibrium, and 3 mL samples are sucked by a syringe every 10 min and are sequenced. Then the xenon lamp is turned on for illumination, and the illumination time is 60 min. During which 3 mL samples were aspirated every 10 min a by syringe and ordered. After sampling, the absorbance of the methylene blue stock solution and the above sample was measured at 664 nm wavelength with an ultraviolet spectrophotometer.
In the experiment, GCN-0 represents original carbon nitride, and GCN-0.5, GCN-1, GCN-2, GCN-3 and GCN-5 represent modified carbon nitrides with xenon lamp illumination of 0.5, 1,2, 3 and 5h respectively.
FIG. 1 shows XPS spectra C1 s, N1 s and O1 s spectra of GCN-0, GCN-2 and GCN-5; as can be seen from FIG. 1, the hydroxyl-OH functional groups in GCN-2 were greatly increased by illumination with ultrapure water for 2h; when the ultrapure water was irradiated with 5 h, the hydroxyl-OH function was restored to the same level as the untreated original GCN.
FIG. 2 shows PL spectra (a) and time resolved photoluminescence spectra (b) of GCN-0, GCN-2 and GCN-5; as can be seen from FIG. 2, the photo-generated carrier recombination rate of GCN-2 is reduced by illumination of ultrapure water for 2h, the life of photo-generated electrons is prolonged, and the photo-generated carrier separation efficiency is higher.
FIG. 3 shows the photocatalytic methylene blue-adsorbing decolorizing performance (a) and the first-order reaction kinetics fitting curve (b) of GCN synthesized under different ultrapure water illumination conditions; as can be seen from FIG. 3, the irradiation of ultrapure water for 2 hours resulted in GCN-2 (99.6%) having a higher photocatalytic adsorption decoloring efficiency and a larger reaction rate constant than GCN (92.0%) which had not been modified by treatment.
FIG. 4 is a graph showing the synthesized GCN photocurrent spectrum under different ultra pure water illumination conditions; as can be seen from FIG. 4, the intensity of the photocurrent of GCN-2 was highest when the ultrapure water was irradiated for 2 hours. And the intensity of the photocurrent of the carbon nitride after being subjected to pure water illumination treatment is higher than that of the original carbon nitride.
In summary, urea is used as a raw material, and the traditional carbon nitride is placed in ultrapure water and light source illumination is applied to change the structure of the carbon nitride, so that hydroxyl-OH functional groups are increased, and modified carbon nitride (GCN) with negative charges on the surface is obtained; meanwhile, the band gap is reduced, the separation efficiency of the photogenerated carriers is greatly improved, and the defects of narrow visible light response range, high electron-hole recombination rate, low carrier transmission efficiency and the like of the traditional g-C 3N4 are effectively overcome. Compared with the traditional physical, chemical and biological means, the method is very suitable for the adsorption and decoloration treatment of high-concentration cationic dye wastewater, uniformly mixes the photocatalyst and the dye wastewater, has obvious decoloration effect in very short time due to the electrostatic adsorption effect under the condition of visible light, and has the advantages of simple treatment process, mild reaction condition, quick degradation, high efficiency and no secondary pollution.
The above embodiments are only for illustrating the technical solution of the present invention, and not for limiting the same; although the invention has been described in detail with reference to the foregoing embodiments, those skilled in the art may still make modifications to the technical solutions described in the foregoing embodiments, or may make equivalent substitutions for some or all of the technical features thereof; such modifications and substitutions do not depart from the spirit of the invention, and are intended to be included within the scope of the appended claims and description.
Claims (9)
1. A simple preparation method of modified carbon nitride is characterized in that:
S1, putting urea into a baking oven to obtain dry urea;
s2, placing the dried urea into a crucible with a cover for calcination to obtain original carbon nitride;
S3, placing the original carbon nitride into ultrapure water, applying xenon lamp illumination for 0.5-5 h, filtering and vacuum drying to obtain the modified carbon nitride.
2. The method for preparing simple modified carbon nitride according to claim 1, wherein the oven drying temperature in step S1 is 105 ℃ and the drying time is 12 h.
3. The method for preparing simple modified carbon nitride according to claim 1, wherein the amount of the added dry urea in step S2 is 30 g, the volume of the crucible used is 30 mL, and the outside is covered with tinfoil; the calcination temperature was 550 ℃, the calcination time was 1h, and the temperature rise rate was 2.5 ℃/min.
4. The method for preparing simple modified carbon nitride according to claim 1, wherein the amount of added original carbon nitride is 0.1 g and the ultrapure water is 200 mL in S3; the drying temperature was 60℃and the time was 12 h.
5. Use of the modified carbon nitride produced by the production method according to any one of claims 1 to 4 for photocatalytic adsorption decolorization of high concentration cationic dye wastewater.
6. The use of modified carbon nitride according to claim 5, wherein a certain amount of modified carbon nitride photocatalyst is taken and put into a condensing beaker, and the modified carbon nitride photocatalyst is uniformly dispersed in a certain concentration volume of methylene blue aqueous solution by ultrasound; before photoreaction, covering the solution with a closed paper box to simulate a dark environment, continuously stirring to reach adsorption and desorption equilibrium, and sucking a sample by using a syringe and sequencing; then, a xenon lamp is turned on for illumination, and the top of the beaker is covered by quartz glass to prevent the liquid from heating and volatilizing; during the process, taking samples by using a syringe and a filter membrane, and sequencing; after sampling, absorbance values of the methylene blue stock solution and the above samples were measured with an ultraviolet spectrophotometer.
7. The use of modified carbon nitride according to claim 6, wherein the amount of the modified carbon nitride photocatalyst added is 0.2 g, the high-concentration dye wastewater is 50 mg/L methylene blue aqueous solution, and the volume is 200 mL.
8. The use of modified carbon nitride according to claim 6, wherein the dark reaction adsorption/desorption time is 30 min, the illumination time is 60 min, the interval sampling time is 10min, and the sampling volume is 3 mL each time.
9. The use of modified carbon nitride according to claim 6, wherein the aqueous methylene blue solution has an ultraviolet test wavelength of 664 nm.
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| US10532939B2 (en) * | 2017-04-19 | 2020-01-14 | King Abdulaziz University | Composite, a method of making thereof, and a method for degrading a pollutant |
| CN107381520A (en) * | 2017-08-24 | 2017-11-24 | 南昌航空大学 | A kind of band gap is adjustable and the preparation method of the class graphene carbonitride of efficient degradation of organic dye |
| CN107803216A (en) * | 2017-10-26 | 2018-03-16 | 苏州大学 | Load hollow mesoporous azotized carbon nano ball composite of bromination Nano silver grain and preparation method thereof and the application in degradation of dye |
| CN108543544B (en) * | 2018-04-28 | 2021-01-01 | 苏州大学 | Honeycomb homoheterojunction carbon nitride composite material, preparation method thereof and application thereof in catalytic treatment of waste gas |
| CN111167496B (en) * | 2020-01-09 | 2020-12-25 | 南开大学 | Visible light catalytic material and preparation method and application thereof |
| CN112121842A (en) * | 2020-10-13 | 2020-12-25 | 南通职业大学 | Carbon nitride quantum dot/tungsten trioxide composite photocatalytic material and preparation method thereof |
| CN113842938A (en) * | 2021-09-18 | 2021-12-28 | 河北零点新能源科技有限公司 | Novel g-C3N4Method for preparing derived carbonaceous adsorbent and photocatalytic material |
| CN115722245A (en) * | 2022-10-18 | 2023-03-03 | 中南林业科技大学 | Defect-state carbon nitride composite photocatalytic material for water body restoration and preparation method thereof |
-
2023
- 2023-10-08 CN CN202311292768.6A patent/CN117205956B/en active Active
Non-Patent Citations (1)
| Title |
|---|
| 真空加热和电子束辐照改性处理g-C3N4光催化剂;张云龙 等;上海大学学报;20170630;第23卷(第3期);1.2 典型g-C3N4的合成、1.3 两种改性后处理方法 * |
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