CN110142055B - Microwave irradiation method for enhancing photocatalytic performance of graphite-phase carbon nitride - Google Patents
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/24—Nitrogen compounds
-
- B01J35/39—
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/34—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation
- B01J37/341—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation
- B01J37/344—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation of electromagnetic wave energy
- B01J37/346—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation of electromagnetic wave energy of microwave energy
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/308—Dyes; Colorants; Fluorescent agents
Abstract
The invention discloses a microwave irradiation method for enhancing the photocatalytic performance of graphite-phase carbon nitride, which comprises the following steps: uniformly dispersing graphite-phase carbon nitride into ethanol to obtain a precursor ethanol mixture, and performing microwave irradiation on the precursor ethanol mixture in a microwave oven for N minutes to obtain modified graphite-phase carbon nitride, wherein N is 1-5, and the power of the microwave irradiation is 800-1000W; the ratio of the mass of the graphite-phase carbon nitride to the volume of the ethanol is 5 (1-4). The microwave irradiation method can simply and efficiently improve the catalytic efficiency of the graphite-phase carbon nitride, achieves the effect of quickly decomposing organic pollutants under the irradiation of visible light, has simple process and no pollution in the preparation process, and has important significance for the research on the photocatalytic performance of the carbon nitride material.
Description
Technical Field
The invention belongs to the technical field of preparation and application of catalytic materials, and particularly relates to a microwave irradiation method for enhancing the photocatalytic performance of graphite-phase carbon nitride.
Background
In modern society, environmental pollution becomes a considerable problem, especially water pollution, which causes great harm to people's life. Conventionally, various measures are taken to treat polluted water, such as new inorganic non-metal catalysis, wherein graphite phase carbon nitride has the advantages of high efficiency, simplicity and the like, and has excellent pollutant degradation capability under the irradiation of visible light. The layered stacking structure of graphite-phase carbon nitride is similar to that of graphite, and the electronic band structure of the graphite-phase carbon nitride enables the graphite-phase carbon nitride to have excellent catalytic performance, including photocatalytic degradation of organic pollutants and hydrogen production through water photolysis. In order to further improve the catalytic performance of graphite-phase carbon nitride, various methods for modifying the graphite-phase carbon nitride are available, including conventional methods such as compounding and doping metal ions, and methods such as morphological change and surface treatment. Although the graphite phase carbon nitride is an inorganic non-metal catalyst with good performance at the present stage, the catalytic efficiency of the graphite phase carbon nitride still has room for improvement.
Disclosure of Invention
The invention aims to overcome the defects of the prior art and provide a microwave irradiation method for enhancing the photocatalytic performance of graphite-phase carbon nitride, and the microwave irradiation method can simply and efficiently improve the catalytic efficiency of the graphite-phase carbon nitride.
Another object of the present invention is to provide a modified graphite phase carbon nitride.
The invention also aims to provide application of the microwave irradiation method in enhancing the photocatalytic performance of graphite-phase carbon nitride.
The invention is realized by the following technical scheme:
a microwave irradiation method for enhancing the photocatalytic performance of graphite-phase carbon nitride comprises the following steps:
uniformly dispersing graphite-phase carbon nitride into ethanol to obtain a precursor ethanol mixture, and performing microwave irradiation on the precursor ethanol mixture in a microwave oven for N minutes to obtain modified graphite-phase carbon nitride, wherein N is 1-5, and the power of the microwave irradiation is 800-1000W; the ratio of the mass of the graphite-phase carbon nitride to the volume of the ethanol is 5 (1-4).
In the above technical solution, the microwave oven is a household microwave oven.
In the above technical solution, the unit of the mass is g, and the unit of the volume is L.
In the technical scheme, when N is more than 1, the microwave irradiation for N minutes is carried out intermittently for N times, the microwave irradiation is suspended after 1 minute of each microwave irradiation, and the microwave irradiation is continued after the precursor ethanol mixture is cooled to the room temperature of 20-25 ℃ along with the furnace until the total microwave irradiation time reaches N minutes.
In the above technical scheme, the preparation method of the graphite phase carbon nitride comprises the following steps: heating melamine, urea, dicyanodiamide or thiourea from the room temperature of 20-25 ℃ to the temperature of 550-600 ℃ in an air environment, and preserving the heat for 2-3 hours to obtain the graphite-phase carbon nitride, wherein the heating rate is 2-10 ℃/min.
The modified graphite-phase carbon nitride is obtained by the microwave irradiation method.
The microwave irradiation method is applied to enhancing the photocatalytic performance of graphite-phase carbon nitride.
The modified graphite phase carbon nitride is applied to shortening the photocatalysis time.
In the technical scheme, the modified graphite-phase carbon nitride is added into a dye solution and irradiated by visible light, and after degradation is carried out for 10min, the residual rate of the dye in the dye solution is less than 20%; when degraded to 15min, the dye was completely degraded.
In the above technical scheme, the dye is rhodamine B, and the ratio of the mass of the modified graphite-phase carbon nitride to the concentration of the dye solution is 0.1: 20, the unit of the mass is g, and the unit of the concentration is mg/L.
Compared with the prior art, the microwave irradiation method can simply and efficiently improve the catalytic efficiency of the graphite-phase carbon nitride, achieves the effect of quickly decomposing organic pollutants under the irradiation of visible light, has simple process and no pollution in the preparation process, and has important significance for the research on the photocatalytic performance of the carbon nitride material.
Drawings
FIG. 1 is an XRD diffraction pattern of graphite phase carbon nitride and modified graphite phase carbon nitride;
FIG. 2 is an FTIR spectrum of graphite phase carbon nitride and modified graphite phase carbon nitride;
FIG. 3 is a BET plot of graphite phase carbon nitride and modified graphite phase carbon nitride;
FIG. 4 is an SEM and TEM of graphite phase carbon nitride and modified graphite phase carbon nitride;
FIG. 5 is a graph of photodegradation rhodamine B performance of graphite phase carbon nitride and modified graphite phase carbon nitride.
Detailed Description
In order to make the present invention/invention scheme better understood by those skilled in the art, the technical scheme of the present invention is further described below with reference to the accompanying drawings and specific embodiments.
In a particular embodiment of the invention, urea CO (NH)2)2Purchased from Henshan chemical, rhodamine B (RhB) C28H37ClN2O3Purchased from Fuchen chemical reagent plant, Tianjin, ethanol C2H6O purchased from Hengshan chemical industry, and the above reagents were all analytically pure.
The microwave oven is a household microwave oven, and the specific model is KD21C, AN (B);
the XRD test instrument and model are as follows: x-ray powder diffractometer, RINT Ultima-III, Rigaku, Japan;
the SEM test instruments and models were: scanning Electron microscope, S-4800, Hitachi, Japan;
the TEM test instrument and model are as follows: high resolution transmission electron microscopy, JEM-6700F, Hitachi, Japan;
the measuring instrument and model of FTIR spectrum are: fourier Infrared Spectroscopy, WQE-410, Bruker, USA;
the test instrument and model of the BET spectrum are as follows: a fully automatic physical chemical adsorption apparatus, AUTOSORB-1, american kanta corporation;
the test instrument and the model of the photodegradation rhodamine B performance diagram are as follows: ultraviolet visible spectrophotometer, TU-1901, beijing general analysis instruments ltd; the method for testing the photodegradation rhodamine B performance graph comprises the following steps: preparing 20mg/L rhodamine B solution, taking 100ml of the rhodamine B solution as a simulated pollutant, taking 0.1g of a sample to be tested (graphite-phase carbon nitride and modified graphite-phase carbon nitride) and putting the sample into the simulated pollutant, performing shading dark treatment (wrapping a beaker by tinfoil), performing magnetic stirring for 40min, taking a sample once after reaching adsorption balance (sampling about 7ml of upper-layer solution, setting the irradiation time to be 0at the moment), starting testing, irradiating by visible light (more than or equal to 420nm) (simultaneously performing magnetic stirring), finishing the illumination for 30min, wherein sampling once every 5min, centrifuging the 7 samples (including 6 times in the testing process and 1 time before the testing), taking upper-layer clarified liquid to test the ultraviolet-visible absorption full-wave scanning spectrum of the upper-layer clarified liquid, and taking the data at 554nm as the absorbance of the rhodamine B. The absorbance of (residual) rhodamine B in 6 times of samples in the test process is respectively compared with the absorbance of rhodamine B in 1 time of samples before the test (namely, initial solution), namely the residual rate of the dye.
Organic contaminants degraded by graphite phase carbon nitride and modified graphite phase carbon nitride can be simulated using rhodamine B or methyl orange.
Example 1
A microwave irradiation method for enhancing the photocatalytic performance of graphite-phase carbon nitride comprises the following steps:
uniformly dispersing faint yellow powdery graphite phase carbon nitride into ethanol to obtain a precursor ethanol mixture, performing microwave irradiation on the precursor ethanol mixture in a microwave oven for 4 minutes to obtain modified graphite phase carbon nitride, wherein the 4-minute microwave irradiation is performed at 4 intervals, the microwave irradiation is suspended after 1 minute of each microwave irradiation, and the microwave irradiation is continued until the whole microwave irradiation time reaches 4 minutes after the precursor ethanol mixture is cooled to the room temperature of 20-25 ℃ along with the oven; the power of microwave irradiation is 800W; the mass of the graphite phase carbon nitride was 0.5g, and the volume of ethanol was 200 mL.
The preparation method of the graphite phase carbon nitride comprises the following steps: and (2) putting urea serving as a precursor into a corundum crucible, putting the crucible into a muffle furnace in an air environment, heating the urea from the room temperature of 20-25 ℃ to 550 ℃, and preserving the heat for 3 hours to obtain the graphite-phase carbon nitride, wherein the heating rate is 10 ℃/min.
FIG. 1 is an XRD diffraction pattern of graphite phase carbon nitride and modified graphite phase carbon nitride in example 1, and it can be seen that the modified graphite phase carbon nitride is carbon nitride, wherein MT-g-C3N4For modifying graphite-phase carbon nitride, g-C3N4Is graphite phase carbon nitride.
FIG. 2 shows an embodimentFTIR spectra of graphite phase carbon nitride and modified graphite phase carbon nitride of 1, wherein MT-g-C3N4For modifying graphite-phase carbon nitride, g-C3N4Is graphite phase carbon nitride. As can be seen from the figure, the absorbance of-OH groups of the modified graphite-phase carbon nitride after the microwave treatment was increased, indicating that the surface hydroxyl group content of the graphite-phase carbon nitride after the microwave treatment was increased.
FIG. 3 is a BET plot of the graphite phase carbon nitride and the modified graphite phase carbon nitride of example 1, wherein MT-g-C3N4For modifying graphite-phase carbon nitride, g-C3N4Is graphite phase carbon nitride. As can be seen from the figure, the specific surface area and the porosity of the modified graphite-phase carbon nitride after microwave treatment are both improved, and the specific surface area is 66.7m2The volume/g (graphite phase carbon nitride) is increased to 72.5m2(modified graphite phase carbon nitride).
Fig. 4 is SEM and TEM spectra of graphite phase carbon nitride and modified graphite phase carbon nitride in example 1, where fig. 4(a) is SEM of graphite phase carbon nitride, fig. 4(b) is SEM of modified graphite phase carbon nitride, fig. 4(c) is TEM of graphite phase carbon nitride, and fig. 4(d) is TEM of modified graphite phase carbon nitride. As can be seen, the modified graphite phase carbon nitride lamellar structure becomes thinner and porous.
EDX elemental analysis showed that g-C3N4(C/N1.40, O1.40 at%) with a C/N molar ratio and an O content lower than MT-g-C3N4(C/N. RTM.1.51, O. RTM.3.25 at%), indicating MT-g-C3N4Nitrogen vacancy defects may be formed in the (modified graphite phase carbon nitride) framework, or microwave bombardment may cause C-NH2Conversion of the terminal groups to C-OH groups.
Example 2
A microwave irradiation method for enhancing the photocatalytic performance of graphite-phase carbon nitride comprises the following steps:
uniformly dispersing faint yellow powdery graphite phase carbon nitride into ethanol to obtain a precursor ethanol mixture, performing microwave irradiation on the precursor ethanol mixture in a microwave oven for 3 minutes to obtain modified graphite phase carbon nitride, wherein the microwave irradiation for 3 minutes is performed at intervals of 3 times, the microwave irradiation is suspended after 1 minute of each microwave irradiation, and the microwave irradiation is continued until the whole microwave irradiation time reaches 3 minutes after the precursor ethanol mixture is cooled to the room temperature of 20-25 ℃ along with the oven; the power of microwave irradiation is 800W; the mass of the graphite phase carbon nitride was 0.5g, and the volume of ethanol was 200 mL.
The preparation method of the graphite phase carbon nitride is a thermal polycondensation method, and specifically comprises the following steps: and (2) putting urea into a corundum crucible, putting the crucible into a muffle furnace in an air environment, heating the urea from the room temperature of 20-25 ℃ to 550 ℃, and preserving the heat for 3 hours to obtain graphite-phase carbon nitride, wherein the heating rate is 10 ℃/min.
Example 3
A microwave irradiation method for enhancing the photocatalytic performance of graphite-phase carbon nitride comprises the following steps:
uniformly dispersing faint yellow powdery graphite phase carbon nitride into ethanol to obtain a precursor ethanol mixture, and performing microwave irradiation on the precursor ethanol mixture in a microwave oven for 5 minutes to obtain modified graphite phase carbon nitride, wherein the microwave irradiation for 5 minutes is performed for 5 times intermittently, the microwave irradiation is suspended after 1 minute of each microwave irradiation, and the microwave irradiation is continued until the whole microwave irradiation time reaches 5 minutes after the precursor ethanol mixture is cooled to the room temperature of 20-25 ℃ along with the oven; the power of microwave irradiation is 800W; the mass of the graphite phase carbon nitride was 0.5g, and the volume of ethanol was 200 mL.
The preparation method of the graphite phase carbon nitride comprises the following steps: and (2) putting urea into a corundum crucible, putting the crucible into a muffle furnace in an air environment, heating the urea from the room temperature of 20-25 ℃ to 550 ℃, and preserving the heat for 3 hours to obtain graphite-phase carbon nitride, wherein the heating rate is 10 ℃/min.
Fig. 5 is a graph of the performance of photodegradation rhodamine B of graphite-phase carbon nitride and modified graphite-phase carbon nitride in examples 1-3 (a visible light source is replaced by a xenon lamp with a 420nm cut-off filter, and the organic pollutant is rhodamine B), wherein curve 1 is an adsorption equilibrium blank control, that is, the sample prepared in example 1 is added into a rhodamine B solution, and no illumination is performed, which proves that the disappearance effect of other curve dyes is generated by degradation rather than adsorption. Curve 2 is a photo-degradable rhodamine B performance map of graphite-phase carbon nitride, curve 3 is a photo-degradable rhodamine B performance map of modified graphite-phase carbon nitride obtained in example 2, curve 4 is a photo-degradable rhodamine B performance map of modified graphite-phase carbon nitride obtained in example 1, and curve 5 is a photo-degradable rhodamine B performance map of modified graphite-phase carbon nitride obtained in example 3. It can be seen from the figure that, compared with graphite-phase carbon nitride, the photodegradation efficiency of the modified graphite-phase carbon nitride is significantly improved, and the photodegradation efficiency of the modified graphite-phase carbon nitride after 4 minutes of microwave irradiation is the highest, and when the modified graphite-phase carbon nitride prepared in example 1 is degraded for 10 minutes, the residual rate of the dye (rhodamine B) in the solution is less than 20% (compared with the amount of the rhodamine B before the start of irradiation), and the modified graphite-phase carbon nitride is completely degraded in 15 minutes. In other examples, the dye is completely degraded for at least 20min, and the original graphite phase carbon nitride is degraded only in 30 min. The microwave irradiation improves the separation efficiency of photon-generated carriers and promotes the absorption and reaction capacity of organic pollutants on the surface.
The invention/invention has been described above by way of example, and it should be noted that any simple variation, modification or other equivalent replacement by a person skilled in the art without any inventive step may fall within the scope of protection of the invention/invention without departing from the core of the invention.
Claims (5)
1. A microwave irradiation method for enhancing the photocatalytic performance of graphite-phase carbon nitride is characterized by comprising the following steps:
uniformly dispersing graphite-phase carbon nitride into ethanol to obtain a precursor ethanol mixture, and performing microwave irradiation on the precursor ethanol mixture in a microwave oven for N minutes to obtain modified graphite-phase carbon nitride, wherein N = 1-5, and the power of the microwave irradiation is 800-1000W; and the ratio of the mass of the graphite-phase carbon nitride to the volume of the ethanol is 5 (1-4), the unit of the mass is g, the unit of the volume is L, when the N is more than 1, the microwave irradiation for N minutes is carried out for N times intermittently, the microwave irradiation is suspended after 1 minute of microwave irradiation, and the microwave irradiation is continued until the total microwave irradiation time reaches N minutes after the precursor ethanol mixture is cooled to the room temperature of 20-25 ℃ along with the furnace.
2. The microwave irradiation method according to claim 1, wherein the preparation method of the graphite-phase carbon nitride comprises: heating melamine, urea, dicyanodiamide or thiourea from the room temperature of 20-25 ℃ to the temperature of 550-600 ℃ in an air environment, and preserving the heat for 2-3 hours to obtain the graphite-phase carbon nitride, wherein the heating rate is 2-10 ℃/min.
3. A microwave irradiation method as claimed in claim 2, wherein said microwave oven is a household microwave oven.
4. The modified graphite-phase carbon nitride obtained by the microwave irradiation method according to claim 1 or 2.
5. The application of the microwave irradiation method in enhancing the photocatalytic performance of graphite-phase carbon nitride according to any one of claims 1 to 3, wherein the modified graphite-phase carbon nitride is added into a dye solution and is irradiated by visible light, and after 10min of degradation, the residual rate of the dye in the dye solution is less than 20%; when degraded to 15min, the dye was completely degraded.
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| CN102266766A (en) * | 2011-05-17 | 2011-12-07 | 内蒙古大学 | Method for microwave-assisted preparation of high-efficient visible-light photocatalysis material |
| CN105148973A (en) * | 2015-09-17 | 2015-12-16 | 上海大学 | Preparation method for electron beam irradiation modified graphite-like-phase carbon nitride for visible-light-driven photocatalyst |
| CN105854922A (en) * | 2016-04-25 | 2016-08-17 | 陕西科技大学 | Mpg-C3N4 photocatalyst with high photocatalytic activity and preparation method and application thereof |
| CN106542509A (en) * | 2016-10-19 | 2017-03-29 | 张家港市东大工业技术研究院 | A kind of efficient method for preparing class Graphene carbonitride |
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