CN112023965A - Regulation and control g-C3N4Method for producing crystallinity - Google Patents
Regulation and control g-C3N4Method for producing crystallinity Download PDFInfo
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- 230000033228 biological regulation Effects 0.000 title claims description 5
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 17
- 238000002360 preparation method Methods 0.000 claims abstract description 16
- 238000000034 method Methods 0.000 claims abstract description 12
- WCUXLLCKKVVCTQ-UHFFFAOYSA-M Potassium chloride Chemical compound [Cl-].[K+] WCUXLLCKKVVCTQ-UHFFFAOYSA-M 0.000 claims description 54
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 29
- 235000011164 potassium chloride Nutrition 0.000 claims description 27
- 239000001103 potassium chloride Substances 0.000 claims description 27
- 238000001354 calcination Methods 0.000 claims description 20
- 229910052573 porcelain Inorganic materials 0.000 claims description 20
- ZFSLODLOARCGLH-UHFFFAOYSA-N isocyanuric acid Chemical compound OC1=NC(O)=NC(O)=N1 ZFSLODLOARCGLH-UHFFFAOYSA-N 0.000 claims description 17
- 229920000877 Melamine resin Polymers 0.000 claims description 15
- JDSHMPZPIAZGSV-UHFFFAOYSA-N melamine Chemical compound NC1=NC(N)=NC(N)=N1 JDSHMPZPIAZGSV-UHFFFAOYSA-N 0.000 claims description 15
- 238000010438 heat treatment Methods 0.000 claims description 13
- 238000001035 drying Methods 0.000 claims description 12
- 230000001699 photocatalysis Effects 0.000 claims description 11
- 239000012300 argon atmosphere Substances 0.000 claims description 9
- 239000008367 deionised water Substances 0.000 claims description 8
- 229910021641 deionized water Inorganic materials 0.000 claims description 8
- 238000004519 manufacturing process Methods 0.000 claims description 8
- 239000000463 material Substances 0.000 claims description 7
- 238000007146 photocatalysis Methods 0.000 claims description 2
- 150000001875 compounds Chemical class 0.000 claims 1
- 239000011941 photocatalyst Substances 0.000 abstract description 22
- 229910052739 hydrogen Inorganic materials 0.000 abstract description 20
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 abstract description 17
- 239000001257 hydrogen Substances 0.000 abstract description 17
- 239000013078 crystal Substances 0.000 abstract description 11
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- 230000001276 controlling effect Effects 0.000 abstract description 3
- 239000003054 catalyst Substances 0.000 description 15
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- 238000004140 cleaning Methods 0.000 description 6
- 238000000926 separation method Methods 0.000 description 6
- 101001027838 Pseudonaja textilis Venom prothrombin activator pseutarin-C non-catalytic subunit Proteins 0.000 description 5
- 238000010586 diagram Methods 0.000 description 5
- 238000005516 engineering process Methods 0.000 description 5
- 238000000227 grinding Methods 0.000 description 5
- 230000005540 biological transmission Effects 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 4
- 229910052757 nitrogen Inorganic materials 0.000 description 4
- 241000282414 Homo sapiens Species 0.000 description 3
- 229910052799 carbon Inorganic materials 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- NQTSTBMCCAVWOS-UHFFFAOYSA-N 1-dimethoxyphosphoryl-3-phenoxypropan-2-one Chemical compound COP(=O)(OC)CC(=O)COC1=CC=CC=C1 NQTSTBMCCAVWOS-UHFFFAOYSA-N 0.000 description 2
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- 238000010521 absorption reaction Methods 0.000 description 2
- 125000003277 amino group Chemical group 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
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- 231100000252 nontoxic Toxicity 0.000 description 2
- 230000003000 nontoxic effect Effects 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 238000013032 photocatalytic reaction Methods 0.000 description 2
- 229910052700 potassium Inorganic materials 0.000 description 2
- 238000000101 transmission high energy electron diffraction Methods 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 238000004435 EPR spectroscopy Methods 0.000 description 1
- GSEJCLTVZPLZKY-UHFFFAOYSA-N Triethanolamine Chemical compound OCCN(CCO)CCO GSEJCLTVZPLZKY-UHFFFAOYSA-N 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
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- 238000000354 decomposition reaction Methods 0.000 description 1
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- 239000000446 fuel Substances 0.000 description 1
- 238000004817 gas chromatography Methods 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
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- 238000002329 infrared spectrum Methods 0.000 description 1
- 230000031700 light absorption Effects 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- JMANVNJQNLATNU-UHFFFAOYSA-N oxalonitrile Chemical compound N#CC#N JMANVNJQNLATNU-UHFFFAOYSA-N 0.000 description 1
- 231100000719 pollutant Toxicity 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
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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
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/30—Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
- B01J35/39—Photocatalytic properties
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/04—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of inorganic compounds, e.g. ammonia
- C01B3/042—Decomposition of water
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/02—Processes for making hydrogen or synthesis gas
- C01B2203/0266—Processes for making hydrogen or synthesis gas containing a decomposition step
- C01B2203/0277—Processes for making hydrogen or synthesis gas containing a decomposition step containing a catalytic decomposition step
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/10—Catalysts for performing the hydrogen forming reactions
- C01B2203/1041—Composition of the catalyst
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
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Abstract
The invention relates to a photocatalyst, in particular to a preparation method for regulating and controlling the crystallinity of g-C3N 4. Successfully aligning g-C by using simple template method3N4The crystallinity of the crystal is regulated and controlled to prepare g-C with proper crystallinity3N4Photocatalyst (CMCCN-5), and the prepared crystallinity-optimized g-C3N4The photocatalyst is applied to the preparation of hydrogen by decomposing water under visible light.
Description
Technical Field
The invention relates to a photocatalyst for preparing hydrogen by decomposing water under visible light, which successfully pairs g-C by using a simple template method3N4The crystallinity of the crystal is regulated and controlled to prepare g-C with proper crystallinity3N4Photocatalyst (CMCCN-5), and the prepared crystallinity-optimized g-C3N4The photocatalyst is applied to the preparation of hydrogen by decomposing water under visible light.
Background
With the large consumption of fossil fuels and the continuous development of modern industry, the lack of energy has become a major problem restricting the development of human socioeconomic development in the 21 st century. In addition, the problem of the huge pollution caused by the combustion of fossil fuels has brought about a serious disaster to human beings. Therefore, from the perspective of long-term and sustainable development of human society, there is an urgent need to develop an environmentally friendly and renewable technology that can be used for green production of energy and solving environmental problems. Among the many strategies proposed, photocatalytic technology, which has the advantages of economy, cleanliness, safety and sustainability, is considered to be an effective way to address energy shortages and environmental issues. In the presence of a photocatalyst, the photocatalytic technology can convert solar energy into clean chemical energy (hydrogen) which can be directly utilized; in addition, the photocatalysis technology can fully and effectively degrade pollutants in the environment into nontoxic and harmless substances through a green and environment-friendly chemical process.
In recent years, non-metallic polymers-class g-C3N4The material is cheap, the preparation is simple, the material is driven by visible light (the band gap is about 2.7eV), the material is non-toxic, and the material has a series of advantages of unique electronic energy band structure, excellent physical and chemical stability and the like, thereby gaining wide attention in scientific research. Despite the advantages mentioned above, for simple, unmodified g-C3N4For the photocatalyst, the advantage of the photocatalyst still cannot make up for the fact that the separation efficiency of the photogenerated carriers in the photocatalytic reaction is low, and the low charge separation efficiency directly causes the low photocatalytic performance of the photocatalyst and can not reach the standard of practical application. The main reason for these defects is the bulk g-C3N4Is amorphous, and has a large number of carrier recombination centers on the surface, so that the photocatalytic activity of the photocatalyst is low. A great deal of researchers have succeeded in preparing g-C with high crystallinity3N4The photocatalyst has excellent photogenerated carrier separation capacity. However, high crystallinity of g-C3N4The catalyst eliminates a large amount of non-condensed amino groups, so that the catalyst lacks reactive active sites and cannot efficiently utilize photogenerated carriers. Therefore, it is necessary to control g-C3N4The crystallinity of the crystal is optimized, and the high-crystallinity g-C is further improved by constructing more reactive sites3N4The photocatalytic performance of (a).
Disclosure of Invention
The invention aims to provide graphite phase carbon nitride (CMCCN-x) photocatalyst and its preparation method, and application of the photocatalyst in preparing hydrogen by decomposing water under visible light is examined, and g-C3N4The crystallinity is optimized, and more reaction active sites are constructed while the high-efficiency carrier separation capability is kept, so that the prepared CMCCN-5 photocatalyst has higher light utilization rate, and shows excellent performance of decomposing water under visible light to prepare fuel hydrogen.
The present invention achieves the above object by the following technical means.
Regulation and control g-C3N4The preparation method of the crystallinity is characterized by comprising the following steps:
the cyanuric acid, the melamine, the potassium chloride and the absolute ethyl alcohol are ground uniformly, placed in an oven to be dried, then placed in a porcelain boat, then placed in a tubular furnace to be calcined for 1-8 hours under the argon atmosphere, and then cleaned by deionized water and the absolute ethyl alcohol, and dried by the oven.
Further, the mass ratio of cyanuric acid to melamine to potassium chloride is as follows: 1-5: 0.1-3: 0.5-5, the ratio of potassium chloride to absolute ethyl alcohol is 0.5-5 g: 1-3 mL.
Furthermore, the calcination temperature is 500-650 ℃, and the heating rate is 1-10 ℃/min.
Preferably, the mass ratio of cyanuric acid to melamine to potassium chloride is 2.5: 0.5: 2, the ratio of potassium chloride to absolute ethyl alcohol is 2 g: 1mL, the calcining temperature is 550 ℃, the heating rate is 5 ℃/min, and the calcining time is 4 h.
For comparison, bulk phase g-C3N4(PCN) production method
The melamine and the absolute ethyl alcohol are ground uniformly, placed in a drying oven for drying, then placed in a porcelain boat, and then placed in a tube furnace for calcining for 1-8 hours under the argon atmosphere.
Further, the mass of the melamine is 1-8g, and the volume of the absolute ethyl alcohol is 1-3 mL.
Furthermore, the calcination temperature of the tubular furnace is 500-650 ℃, and the heating rate is 1-10 ℃/min.
Preferably, the amount of melamine is 5g, the calcination temperature is 550 ℃, the heating rate is 5 ℃/min, and the calcination time is 4 h.
KCl template method for preparing bulk phase g-C3N4(PCNS) the method is as follows:
the preparation method comprises the steps of grinding melamine, potassium chloride and absolute ethyl alcohol uniformly, placing the ground materials in an oven to be dried, placing the materials in a porcelain boat, then placing the porcelain boat in a tube furnace to be calcined for 1-8 hours under the argon atmosphere, then cleaning the porcelain boat with deionized water and absolute ethyl alcohol, and drying the porcelain boat in the oven.
Further, the mass ratio of melamine to potassium chloride is 1-8: 0.5-5, the ratio of potassium chloride to absolute ethyl alcohol is 0.5-5 g: 1-3 mL.
Furthermore, the calcination temperature of the tubular furnace is 500-650 ℃, and the heating rate is 1-10 ℃/min.
Preferably, the mass ratio of melamine to potassium chloride is 3: 2, the ratio of potassium chloride to absolute ethyl alcohol is 2 g: 1mL, the calcining temperature is 550 ℃, the heating rate is 5 ℃/min, and the calcining time is 4 h.
High crystallinity g-C3N4The preparation method of (CCN) is as follows:
grinding cyanuric acid, potassium chloride and absolute ethyl alcohol uniformly, placing the ground cyanuric acid, potassium chloride and absolute ethyl alcohol into an oven to be dried, placing the ground cyanuric acid, potassium chloride and absolute ethyl alcohol into a porcelain boat, then placing the porcelain boat into a tubular furnace to be calcined for 1-8h under argon atmosphere, then cleaning the porcelain boat with deionized water and absolute ethyl alcohol, and drying the porcelain boat in the oven.
Further, the mass ratio of cyanuric acid to potassium chloride is 1-8: 0.5-5, the ratio of potassium chloride to absolute ethyl alcohol is 0.5-5 g: 1-3 mL.
Furthermore, the calcination temperature of the tubular furnace is 500-650 ℃, and the heating rate is 1-10 ℃/min.
Preferably, the mass ratio of cyanuric acid to potassium chloride is 3: 2, the ratio of potassium chloride to absolute ethyl alcohol is 2 g: 1mL, the calcining temperature is 550 ℃, the heating rate is 5 ℃/min, and the calcining time is 4 h.
The invention has the advantages of
The invention has the advantage of simply and conveniently optimizing g-C3N4And g-C to optimize crystallinity3N4The photocatalyst is used for decomposing water to prepare hydrogen and has good photocatalytic performance. The invention providesThe supplied CMCCN-5 is compared with the conventional g-C3N4The carrier separation is better, the utilization efficiency of photons is higher, so that the high-efficiency photocatalytic activity of the prepared photocatalyst can be exerted, the method does not cause resource waste, is simple and convenient to operate, has lower cost, and is a green and environment-friendly high-efficiency treatment technology.
Drawings
FIG. 1a is an X-ray diffraction pattern at 2 theta of 10 DEG to 40 DEG for the catalyst thus prepared, from which it can be seen that the diffraction peaks at 2 theta of PCN and PCNS at 13 DEG and 27 DEG are observed with amorphous phase g-C3N4The crystal structures of the CMCCN-5 and CCN are obviously changed, while the characteristic peak of the CMCCN-5 and CCN at about 13 ℃ disappears, and the characteristic peak of the (002) crystal face moves from 27 ℃ to 28 ℃. Further comparison of the half-widths of the (002) crystal planes of the prepared samples revealed that the half-widths of CMCCN-5 and CCN were significantly smaller than those of PCN and PCNS in the amorphous phase. FIG. 1b shows that CMCCN-5 and CCN are 10-80 degrees at 2 theta, and the half-width of the (002) crystal face of CMCCN-5 is obviously larger than that of CCN, which shows that the method can effectively change g-C3N4The crystallinity of (a).
FIGS. 2a-f are transmission diagrams of the prepared catalyst: fig. 2a is the SAED and projection diagram of CCN, and it can be seen that there are clearly distributed bright spots in CCN. FIGS. 2b-c are high resolution transmission plots of CCN, where significant lattice fringes can be seen, indicating better crystallinity of CCN. FIG. 2d is a SAED and transmission plot of CMCCN-5, from which the distribution of bright spots cannot be observed. FIGS. 2e-f are high resolution transmission graphs of CMCCN-5, where only some of them are seen to show locally significant lattice fringes, and most of them are random, indicating a significant decrease in crystallinity. The fact that the g-C can be effectively controlled by controlling the amino content of the raw materials is proved by the above3N4The crystallinity of (a). FIG. 2g is a diagram of the distribution of the elements of CMCCN-5, and it can be seen that C, N, O, Cl and K are uniformly distributed.
FIG. 3a is a steady state fluorescence plot of the prepared catalyst, as seen with g-C3N4The improvement in crystallinity, in turn, decreases the intensity of fluorescence. The electrochemical impedance plot of fig. 3b and the transient photocurrent response plot of fig. 3c show similar results to steady state fluorescence. These results show thatg-C3N4The improvement of the crystallinity can effectively enhance the carrier separation capability of the catalyst, and the method is also proved to be capable of effectively regulating and controlling g-C3N4The crystallinity of (a). FIG. 3d is an IR spectrum of the prepared catalyst, which shows that all samples are at 550cm-1To 1800cm-1All show typical g-C3N4Characteristic absorption peak. In addition 3100cm-1Of (a) NH of (b)xThe characteristic peaks of (C) show a clear difference, -NH of the highly crystalline samples (CMCCN-5 and CCN)xThe content is obviously reduced. This indicates-NHxFor g-C3N4Has a critical influence on the formation of crystals. FIG. 3e is an Electron Paramagnetic Resonance (EPR) chart of the prepared sample, showing that the intensity of the formant of the prepared sample is not significantly changed, indicating that the change of the precursor is to g-C3N4The formation of the inner lone pair of electrons has no obvious influence. FIG. 3f is a solid UV diffuse reflectance graph of the prepared catalyst, showing that the maximum absorption wavelength of the prepared catalyst is about 480nm, indicating g-C3N4The crystal regulation and control of the crystal has no obvious influence on the light absorption range of the crystal.
Table 1 is the elemental content table of the prepared catalyst, and it can be seen that the main elements of the prepared catalyst are C, N, H, K, Cl and O. The C, N and H contents of CMCCN-5 and CCN are significantly reduced compared to the PCN and PCNS contents. Further, the N and H content of CMCCN-5 was significantly higher than that of CCN, indicating that more incompletely reacted amine groups were formed in CMCCN-5.
FIG. 4a is a graph of the specific surface area of the prepared catalyst, and it can be seen that the optimized CMCCN-5 shows the maximum specific surface area value, indicating that CMCCN-5 can provide more reactive sites to promote the photocatalytic reaction. FIG. 4b is a plot of the 5 hour hydrogen production of the prepared catalyst, from which it can be seen that CMCCN-5 produces the highest amount of hydrogen at the same time, indicating that CMCCN-5 performs the best. FIG. 4c is a 5h average hydrogen production rate diagram of the prepared catalyst hydrogen production reaction, and the maximum CMCCN-5 value can be seen from the diagram, which shows that the CMCCN-5 has the fastest hydrogen production rate and the best photocatalytic performance. FIG. 4d is a graph of the quantum efficiency of CMCCN-5 under different single-wavelength illumination, and it can be seen that the quantum efficiency of CMCCN-5 at 420nm and 450nm reaches 26.9% and 14.0%, respectively, indicating that it can efficiently convert and utilize absorbed visible light.
Detailed Description
Example 1
Preparation of PCN photocatalyst:
5g of melamine and 1mL of absolute ethyl alcohol are uniformly ground, placed in an oven for drying, then placed in a porcelain boat, then placed in a tube furnace under argon atmosphere, heated to 550 ℃ at the heating rate of 5 ℃/min, and calcined for 4h at 550 ℃. And then, cleaning the mixture by using deionized water and absolute ethyl alcohol, and drying the mixture by using an oven.
Example 2
Preparation of PCNS photocatalyst:
uniformly grinding 3g of melamine, 2g of potassium chloride and 1mL of absolute ethyl alcohol, placing the mixture in an oven for drying, placing the mixture in a porcelain boat, then placing the porcelain boat in a tubular furnace under argon atmosphere, heating to 550 ℃ at the heating rate of 5 ℃/min, and calcining for 4 hours at 550 ℃. And then, cleaning the mixture by using deionized water and absolute ethyl alcohol, and drying the mixture by using an oven.
Example 3
Preparation of CCN photocatalyst:
grinding 3g of cyanuric acid, 2g of potassium chloride and 1mL of absolute ethyl alcohol uniformly, placing the ground cyanuric acid, potassium chloride and absolute ethyl alcohol into an oven for drying, placing the dried cyanuric acid into a porcelain boat, then placing the porcelain boat into a tubular furnace under argon atmosphere, raising the temperature to 550 ℃ at the temperature raising rate of 5 ℃/min, and calcining the porcelain boat for 4 hours at the temperature of 550 ℃. And then, cleaning the mixture by using deionized water and absolute ethyl alcohol, and drying the mixture by using an oven.
Example 4
Preparation of CMCCN-5 photocatalyst (inventive):
grinding 2.5g of cyanuric acid, 0.5g of melamine, 2g of potassium chloride and 1mL of absolute ethyl alcohol uniformly, placing the ground cyanuric acid into an oven to be dried, placing the dried cyanuric acid into a porcelain boat, then placing the porcelain boat into a tubular furnace under argon atmosphere, raising the temperature to 550 ℃ at the temperature raising rate of 5 ℃/min, and calcining the porcelain boat for 4 hours at the temperature of 550 ℃. And then, cleaning the mixture by using deionized water and absolute ethyl alcohol, and drying the mixture by using an oven.
Example 5
The experimental process of photocatalytic water splitting hydrogen production: 0.05g of the catalyst was weighed out and dispersed in 100mL of a solution containing 20% (20mL) triethanolamine and 3 wt% (0.0015g) Pt in 100mL of the solution. Before illumination, argon is introduced into the reaction container, so that air in the reactor is discharged, and the influence of the air on the generation of hydrogen in the water decomposition is avoided. And injecting hydrogen generated by the reaction into the gas chromatography every 1h, and finally calculating the hydrogen yield. As can be seen from FIG. 4b, the prepared CMCCN-5 photocatalyst has excellent activity of producing hydrogen by decomposing water with visible light.
TABLE 1
Claims (5)
1. Regulation and control g-C3N4Method for producing crystallinity by reacting g-C3N4The crystallinity of the compound is optimized, and the g-C is further improved by constructing more reactive sites3N4The photocatalysis performance of the material is characterized in that cyanuric acid, melamine, potassium chloride and absolute ethyl alcohol are ground uniformly, placed in an oven for drying, then placed in a porcelain boat, then placed in a tube furnace for calcining for 1-8h under argon atmosphere, and then cleaned by deionized water and absolute ethyl alcohol, and dried by the oven.
2. The method of claim 1, wherein g-C is modulated3N4The preparation method of the crystallinity is characterized in that the mass ratio of cyanuric acid to melamine to potassium chloride is as follows: 1-5: 0.1-3: 0.5-5, the ratio of potassium chloride to absolute ethyl alcohol is 0.5-5 g: 1-3 mL.
3. The method of claim 1, wherein g-C is modulated3N4The preparation method of the crystallinity is characterized in that the calcination temperature is 500-650 ℃, the heating rate is 1-10 ℃/min, and the calcination time is 4 h.
4. The method of claim 2, wherein g-C is modulated3N4Degree of crystallinityThe preparation method is characterized in that the mass ratio of cyanuric acid to melamine to potassium chloride is 2.5: 0.5: 2, the ratio of potassium chloride to absolute ethyl alcohol is 2 g: 1 mL.
5. The method of claim 3, wherein the g-C is regulated3N4The preparation method of the crystallinity is characterized in that the calcination temperature is 550 ℃, and the heating rate is 5 ℃/min.
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| CN115608401A (en) * | 2022-10-20 | 2023-01-17 | 南京理工大学 | High-crystallinity carbon nitride based on cyanuric acid-lithium chloride eutectic and preparation method thereof |
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