CN110560121B - Method for preparing porous carbon nitride material with assistance of carbon dioxide, porous carbon nitride material and application of porous carbon nitride material - Google Patents
Method for preparing porous carbon nitride material with assistance of carbon dioxide, porous carbon nitride material and application of porous carbon nitride material Download PDFInfo
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- JMANVNJQNLATNU-UHFFFAOYSA-N oxalonitrile Chemical compound N#CC#N JMANVNJQNLATNU-UHFFFAOYSA-N 0.000 title claims abstract description 77
- 239000000463 material Substances 0.000 title claims abstract description 68
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 title claims abstract description 48
- 238000000034 method Methods 0.000 title claims abstract description 33
- 229910002092 carbon dioxide Inorganic materials 0.000 title claims abstract description 24
- 239000001569 carbon dioxide Substances 0.000 title claims abstract description 24
- 238000006243 chemical reaction Methods 0.000 claims abstract description 48
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 21
- 239000008367 deionised water Substances 0.000 claims abstract description 19
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- 229920000877 Melamine resin Polymers 0.000 claims abstract description 16
- JDSHMPZPIAZGSV-UHFFFAOYSA-N melamine Chemical compound NC1=NC(N)=NC(N)=N1 JDSHMPZPIAZGSV-UHFFFAOYSA-N 0.000 claims abstract description 16
- 238000001816 cooling Methods 0.000 claims abstract description 12
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- 238000003760 magnetic stirring Methods 0.000 claims description 5
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- PYWVYCXTNDRMGF-UHFFFAOYSA-N rhodamine B Chemical compound [Cl-].C=12C=CC(=[N+](CC)CC)C=C2OC2=CC(N(CC)CC)=CC=C2C=1C1=CC=CC=C1C(O)=O PYWVYCXTNDRMGF-UHFFFAOYSA-N 0.000 abstract description 16
- 229940043267 rhodamine b Drugs 0.000 abstract description 16
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- XOHRBKMEDWUCCI-UHFFFAOYSA-N carbonic acid;1,3,5-triazine-2,4,6-triamine Chemical compound OC(O)=O.NC1=NC(N)=NC(N)=N1 XOHRBKMEDWUCCI-UHFFFAOYSA-N 0.000 description 2
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- JYEUMXHLPRZUAT-UHFFFAOYSA-N 1,2,3-triazine Chemical group C1=CN=NN=C1 JYEUMXHLPRZUAT-UHFFFAOYSA-N 0.000 description 1
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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—
-
- B01J35/613—
-
- 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
- C02F2101/38—Organic compounds containing nitrogen
Abstract
A method for preparing a porous carbon nitride material with the assistance of carbon dioxide, the porous carbon nitride material and the application thereof adopt a reaction-calcination two-step method, and the preparation steps comprise: weighing and adding metered melamine into a reaction kettle, adding metered deionized water, and introducing carbon dioxide for reaction, wherein the reaction temperature is 50-100 ℃, the reaction pressure is 0.01-1.0 MPa, and the reaction time is 2-6 h; naturally cooling after the reaction is finished, and performing suction filtration to obtain an intermediate; and transferring the intermediate into a crucible with a cover, putting the crucible and the intermediate into a muffle furnace for calcining, heating the muffle furnace to 540-580 ℃ in a furnace cavity at the speed of 2-6 ℃/min, preserving the temperature for 2-5 h, and cooling to room temperature to obtain the porous carbon nitride. The method has the advantages of rich raw material sources, low cost, environmental friendliness, high product yield and simple preparation process; the prepared porous carbon nitride material has large specific surface area and can effectively catalyze photodegradation of rhodamine B.
Description
The technical field of
The invention belongs to the technical field of preparation and application of materials, and particularly relates to a method for preparing a porous carbon nitride material with the aid of carbon dioxide, the porous carbon nitride material and application of the porous carbon nitride material.
Background
The carbon nitride is an inorganic metal material, has high stability, acid and alkali resistance and semiconductor property, and has wide application prospect in the fields of heterogeneous catalysis, fuel cells, gas adsorption and storage and the like. The carbon nitride is prepared by thermal polymerization of nitrogen-containing precursors (such as melamine, dicyandiamide, urea, thiourea, cyanuric acid, etc.). However, the specific surface area and pore volume of carbon nitride prepared by the common thermal polymerization method are small, so that the catalytic performance of the carbon nitride is not high. Increasing the specific surface area of carbon nitride is the key to improving its performance. At present, the methods for preparing carbon nitride with high specific surface area mainly comprise: hard template, soft template, and no template methods.
The hard template method is to use the existing solid as a template, introduce liquid organic precursors such as cyanamide, dicyandiamide and urea into the template, fill the liquid organic precursors into the pores or gaps of the hard template, and remove the template by acid or alkali etching after high-temperature roasting to obtain the porous carbon nitride material (Wangyue, Jianright, ShangZhongkun, Shangjie, LiYongxin. Proc. physico-chemistry report, 2016, 32 (8): 1913-1928). However, the hard template method uses a large amount of acid or alkali for removing the template, which is not environmentally friendly. The soft template method is to use surfactant as soft template, self-assemble the precursor and the soft template to form an ordered structure, decompose the soft template to form a pore channel in the high-temperature polymerization stage, and obtain the porous graphite phase carbon nitride (Lirong, Rongrui, Gonghong, Hengheng. novel chemical material, 2017, 45(1): 35-37.). Compared with the hard template method, the soft template method has the advantages of simple preparation and environmental friendliness, but the soft template has higher price and is not beneficial to large-scale production. The template-free method is to prepare the porous carbon nitride material by using gas released by raw materials in the high-temperature polymerization process as a pore-foaming agent. Urea or thiourea is taken as a raw material and is directly calcined in the air, and a pore structure is formed in a bubbling manner in the gas generated in the calcining process, so that a carbon nitride material (Fanqijing, Liujian army, in the spring, the left victory, the chemical engineering progress 2014, 33 (5): 1185-1194) is obtained, but the product yield is only 4-6% generally by adopting the method, and the product yield is lower. Therefore, the development of a high-efficiency preparation method which has the advantages of simple process, low cost and environmental friendliness is of great significance.
Disclosure of Invention
The invention aims to provide a method for preparing a porous carbon nitride material with the assistance of carbon dioxide, the porous carbon nitride material and application thereof, wherein the method can simplify the preparation process, reduce the production cost and the pollution to the environment and improve the product yield; the prepared porous carbon nitride material has large comparative area and can effectively catalyze photodegradation of rhodamine B.
In order to achieve the aim, the method for preparing the porous carbon nitride material by the aid of the carbon dioxide comprises the following steps:
(1) adding the measured melamine and deionized water into a reaction kettle, starting magnetic stirring, introducing carbon dioxide into the deionized water for reaction, controlling the reaction temperature to be 50-100 ℃, keeping the pressure in the reaction kettle to be 0.01-0.1 MPa, reacting for 2-6 h, naturally cooling after the reaction is finished, and performing suction filtration to obtain an intermediate; the mass ratio of the melamine to the deionized water is 1: (20-100);
(2) and (2) transferring the intermediate obtained in the step (1) into a crucible with a cover, putting the crucible and the crucible into a muffle furnace for calcining, heating the muffle furnace to 540-580 ℃ in a furnace cavity at the speed of 2-6 ℃/min, preserving the temperature for 2-5 h, naturally cooling the temperature in the furnace cavity to room temperature, and taking out the product to obtain the porous carbon nitride.
Preferably, the mass ratio of melamine to deionized water in step (1) is 1: 50.
preferably, in the step (1), the reaction temperature is controlled to be 80 ℃, the pressure in the reaction kettle is 0.05MPa, and the reaction is carried out for 4 hours.
Preferably, in the step (2), the temperature of the muffle furnace is increased to 550 ℃ at the speed of 4 ℃/min, and the temperature is kept for 3 h.
A porous carbon nitride material is prepared by the preparation method.
The porous carbon nitride material prepared by the preparation method is applied to catalytic photodegradation of rhodamine B.
According to the invention, cheap melamine is used as a raw material, carbon dioxide is used as an auxiliary material, water is used as a medium for the raw material and the carbon dioxide to react in a reaction kettle to generate melamine carbonate, the melamine carbonate is continuously decomposed in the calcining process to release carbon dioxide gas to form a pore channel, and meanwhile, the melamine is continuously polymerized to finally form the porous carbon nitride material.
Compared with the prior art, the invention takes cheap and nontoxic carbon dioxide as an auxiliary material and a pore-forming agent, and can obviously reduce the production cost; the carbon dioxide escaping in the calcining process is easy to treat and has little influence on the environment; porous carbon nitride is directly obtained after calcination without post-treatment, so that the production process is simplified; in addition, the yield of the porous carbon nitride material prepared by the method is up to 48%, and the product yield is improved. The invention does not need to use complex and expensive instruments and equipment, and is easy for industrial production. The porous carbon nitride material prepared by the preparation method has large specific surface area, has higher catalytic activity and better repeatability when being used as a catalyst for photodegradation of rhodamine B, and has potential utilization value in the aspect of sewage treatment.
Drawings
FIG. 1 is an X-ray diffraction pattern of a porous carbon nitride material prepared in accordance with example one of the present invention;
FIG. 2 is a scanning electron microscope image of a porous carbon nitride material prepared according to a first embodiment of the present invention;
FIG. 3 is an infrared spectrum of a porous carbon nitride material prepared according to the first embodiment of the present invention;
FIG. 4 is an isothermal adsorption-desorption curve of the porous carbon nitride material prepared in the first embodiment of the present invention;
FIG. 5 is an activity diagram of the porous carbon nitride material prepared in the first embodiment of the invention catalyzing photodegradation of rhodamine B solution;
FIG. 6 is a repeated diagram of the porous carbon nitride material prepared in the first embodiment of the invention catalyzing photodegradation of rhodamine B solution.
Detailed Description
The present invention will be described in further detail with reference to the following drawings and examples.
Example one
A method for preparing a porous carbon nitride material with the assistance of carbon dioxide comprises the following steps:
(1) adding the measured melamine into a reaction kettle, adding the measured deionized water, starting magnetic stirring, introducing carbon dioxide into the deionized water for reaction, controlling the reaction temperature to be 80 ℃, keeping the pressure in the reaction kettle to be 0.05MPa, reacting for 4 hours, naturally cooling after the reaction is finished, and performing suction filtration to obtain an intermediate; the mass ratio of the melamine to the deionized water is 1: 50;
(2) And transferring the intermediate into a crucible with a cover, putting the crucible and the intermediate into a muffle furnace for calcining, heating the muffle furnace to 550 ℃ at the speed of 4 ℃/min, preserving the temperature for 3h, naturally cooling the temperature in the furnace to room temperature, taking out the product to obtain the porous carbon nitride, and obtaining the porous carbon nitride with the yield of 45% by calculation.
The material is characterized by an X-ray diffractometer, a scanning electron microscope, an infrared spectrometer, a physical adsorption apparatus and the like. The X-ray diffraction pattern, the scanning electron microscope pattern, the infrared spectrogram and the isothermal adsorption-desorption curve of the material prepared by the steps are respectively shown in figure 1, figure 2, figure 3 and figure 4.
As can be seen from fig. 1, there are two distinct diffraction peaks at 13.1 ° and 27.1 ° in the figure, which are characteristic peaks of carbon nitride material, corresponding to the (100) and (002) crystal planes of carbon nitride, respectively. The diffraction peak at 27.1 degrees is sharper, which indicates that the crystallinity of the material is higher, and indicates that the prepared sample is a porous carbon nitride material.
As can be seen from fig. 2, the sample prepared in this example is an irregular material piled up in bulk.
As can be seen from FIG. 3, the sample prepared in this example was 1259cm-1、1329cm-1、1405cm-1、1468cm-1And 1580cm-1A stretching vibration peak of 1646cm at C-N bond -1Is characterized in that C is an N bond stretching vibration peak, 813cm-1Is the stretching vibration peak of the triazine ring, 3164cm-1Is located at the stretching vibration peak of O-H and N-H for absorbing water molecules, andthe step shows that the prepared sample is a porous carbon nitride material.
From FIG. 4, it can be calculated that the BET specific surface area of the sample prepared in this example is 48.4m2/g。
A porous carbon nitride material is prepared by the preparation method.
In order to further verify the catalytic performance of the porous carbon nitride material prepared in the embodiment, the porous carbon nitride material prepared in the embodiment is used for catalyzing the reaction of photodegradation of rhodamine B, and the catalytic activity of the porous carbon nitride material is tested. The specific verification process is as follows:
300mL of 10mg/L rhodamine B solution is measured and put into a beaker, 0.3g of the porous carbon nitride material prepared in the embodiment is added, the beaker is put into a photocatalytic reactor, and the light source is a 500W xenon lamp. Firstly carrying out a dark reaction for 1h, namely, carrying out a reaction without turning on a lamp, turning on a xenon lamp to carry out a photocatalytic reaction after the dark reaction is finished, extracting 5mL of liquid by using a needle tube with a filter membrane every 20min, measuring the absorbance of the liquid at 554nm by using an ultraviolet-visible spectrophotometer, and monitoring the reaction process. In addition, a comparative experiment was conducted without adding the porous carbon nitride material, and the rest of the process was the same. After the reaction is finished, the catalyst is centrifugally separated, washed by deionized water for 3 times and then reused, and the repeatability of the material is tested.
Fig. 5 is a graph showing the effect of the porous carbon nitride prepared in this example on catalyzing photodegradation of rhodamine B solution. The upper curve represents the reaction results without adding the carbon nitride material, and the lower curve represents the reaction results with adding the porous carbon nitride material prepared in this example as a catalyst. As can be seen from the figure, the concentration of rhodamine B in the control group has little change after 100min illumination. In the experimental group added with the carbon nitride material, the concentration of rhodamine B is obviously reduced at the initial stage of dark reaction and then is basically unchanged, which shows that the adsorption balance is achieved, the concentration of rhodamine B is gradually reduced after illumination is started, the rhodamine B is basically completely degraded in 100min, and the catalytic effect is obvious.
FIG. 6 is a repetitive histogram of the porous carbon nitride material prepared in this example for catalyzing photodegradation of rhodamine B, from which it can be seen that the activity changes little in the first 6 times and decreases significantly in the 7 th time, indicating that the catalytic activity of the material is relatively stable; after each of the first 6 uses, there was a small decrease in catalytic activity, mainly due to a small loss of the material during the separation process.
Example two
A method for preparing a porous carbon nitride material with the assistance of carbon dioxide comprises the following steps:
(1) Adding the measured melamine into a reaction kettle, adding the measured deionized water, starting magnetic stirring, introducing carbon dioxide into the deionized water for reaction, controlling the reaction temperature to be 50 ℃, keeping the pressure in the reaction kettle to be 0.01MPa, reacting for 6 hours, naturally cooling after the reaction is finished, and performing suction filtration to obtain an intermediate; the mass ratio of the melamine to the deionized water is 1: 100;
(2) and transferring the intermediate into a crucible with a cover, putting the crucible and the intermediate into a muffle furnace for pyrolysis, heating the muffle furnace to 540 ℃ at the speed of 6 ℃/min, preserving the temperature for 5h, naturally cooling the temperature in the furnace to room temperature, taking out the product to obtain the porous carbon nitride, and obtaining the yield of the porous carbon nitride by calculation, wherein the yield of the porous carbon nitride is 43%.
A porous carbon nitride material is prepared by the preparation method.
The results of samples prepared by using the characteristics of an X-ray diffractometer, a scanning electron microscope, an infrared spectrometer, a physical adsorption instrument and the like show that the prepared samples are porous carbon nitride materials, and the specific surface area is 35.4m2/g。
The porous carbon nitride carbon material prepared by the embodiment is used for catalyzing the reaction of photodegradation of rhodamine B, and test results show that the material has high catalytic activity and good repeatability.
EXAMPLE III
A method for preparing a porous carbon nitride material with the assistance of carbon dioxide comprises the following steps:
(1) adding the measured melamine into a reaction kettle, adding the measured deionized water, starting magnetic stirring, introducing carbon dioxide into the deionized water for reaction, controlling the reaction temperature to be 100 ℃, keeping the pressure in the reaction kettle to be 0.1MPa, reacting for 2 hours, naturally cooling after the reaction is finished, and performing suction filtration to obtain an intermediate; the mass ratio of the melamine to the deionized water is 1: 20;
(2) and transferring the intermediate into a crucible with a cover, putting the crucible and the intermediate into a muffle furnace for pyrolysis, heating the muffle furnace to 580 ℃ at the speed of 2 ℃/min, preserving the temperature for 2h, naturally cooling the temperature in the furnace to room temperature, taking out the product to obtain the porous carbon nitride, and obtaining the porous carbon nitride with the yield of 48% by calculation.
A porous carbon nitride material is prepared by the preparation method.
The results of samples prepared by using the characteristics of an X-ray diffractometer, a scanning electron microscope, an infrared spectrometer, a physical adsorption instrument and the like show that the prepared samples are porous carbon nitride materials, and the specific surface area is 42.3m2/g。
The porous carbon nitride carbon material prepared by the embodiment is used for catalyzing the reaction of photodegradation of rhodamine B, and test results show that the material has high catalytic activity and good repeatability.
Claims (5)
1. A method for preparing a porous carbon nitride material with the assistance of carbon dioxide is characterized by comprising the following steps:
(1) adding the measured melamine into a reaction kettle, adding the measured deionized water, starting magnetic stirring, introducing carbon dioxide into the deionized water for reaction, controlling the reaction temperature to be 50-100 ℃, keeping the pressure in the reaction kettle to be 0.01-0.1 MPa, reacting for 2-6 h, naturally cooling after the reaction is finished, and performing suction filtration to obtain an intermediate; the mass ratio of the melamine to the deionized water is 1: (20-100);
(2) and (2) transferring the intermediate obtained in the step (1) into a crucible with a cover, putting the crucible and the crucible into a muffle furnace for calcining, raising the temperature of the muffle furnace to 540-580 ℃ in a furnace cavity at the speed of 2-6 ℃/min, preserving the temperature for 2-5 h, naturally cooling the temperature in the furnace cavity to room temperature, and taking out the product to obtain the porous carbon nitride.
2. The method for preparing the porous carbon nitride material with the assistance of the carbon dioxide as claimed in claim 1, wherein the mass ratio of the melamine to the deionized water in the step (1) is 1: 50.
3. the method for preparing the porous carbon nitride material by the aid of the carbon dioxide according to claim 1 or 2, wherein the reaction temperature in the step (1) is controlled to be 80 ℃, the pressure in the reaction kettle is controlled to be 0.05 MPa, and the reaction is carried out for 4 hours.
4. The method for preparing the porous carbon nitride material by the aid of the carbon dioxide as claimed in claim 1 or 2, wherein in the step (2), the temperature of the muffle furnace is increased to 550 ℃ in the furnace cavity at a speed of 4 ℃/min, and the temperature is kept for 3 hours.
5. A porous carbon nitride material produced by the production method according to any one of claims 1 to 4.
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| "Mesoporous graphitic carbon nitride (g-C3N4) nanosheets synthesized from carbonated beverage-reformed commercial melamine for enhanced photocatalytic hydrogen evolution";Shaodong Sun et al.,;《Mater. Chem. Front.,》;20190131;第3卷;第597-605页 * |
| Shaodong Sun et al.,."Mesoporous graphitic carbon nitride (g-C3N4) nanosheets synthesized from carbonated beverage-reformed commercial melamine for enhanced photocatalytic hydrogen evolution".《Mater. Chem. Front.,》.2019,第3卷第597-605页. * |
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Application publication date: 20191213 Assignee: XUZHOU LANHU INFORMATION TECHNOLOGY Co.,Ltd. Assignor: XUZHOU University OF TECHNOLOGY Contract record no.: X2023320000179 Denomination of invention: A Method for Preparing Porous Carbon Nitride Materials Assisted by Carbon Dioxide and Porous Carbon Nitride Materials and Their Applications Granted publication date: 20220610 License type: Common License Record date: 20230731 |