CN112023965B - Regulation and control g-C 3 N 4 Preparation method of crystallinity - Google Patents
Regulation and control g-C 3 N 4 Preparation method of crystallinity Download PDFInfo
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- 238000002360 preparation method Methods 0.000 title claims abstract description 16
- 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
- 230000001105 regulatory effect Effects 0.000 claims abstract description 5
- WCUXLLCKKVVCTQ-UHFFFAOYSA-M Potassium chloride Chemical compound [Cl-].[K+] WCUXLLCKKVVCTQ-UHFFFAOYSA-M 0.000 claims description 56
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 31
- 235000011164 potassium chloride Nutrition 0.000 claims description 28
- 239000001103 potassium chloride Substances 0.000 claims description 28
- 238000001354 calcination Methods 0.000 claims description 20
- 229910052573 porcelain Inorganic materials 0.000 claims description 18
- 229920000877 Melamine resin Polymers 0.000 claims description 17
- JDSHMPZPIAZGSV-UHFFFAOYSA-N melamine Chemical compound NC1=NC(N)=NC(N)=N1 JDSHMPZPIAZGSV-UHFFFAOYSA-N 0.000 claims description 17
- ZFSLODLOARCGLH-UHFFFAOYSA-N isocyanuric acid Chemical compound OC1=NC(O)=NC(O)=N1 ZFSLODLOARCGLH-UHFFFAOYSA-N 0.000 claims description 16
- 239000012300 argon atmosphere Substances 0.000 claims description 9
- 238000010438 heat treatment Methods 0.000 claims description 9
- 239000008367 deionised water Substances 0.000 claims description 8
- 229910021641 deionized water Inorganic materials 0.000 claims description 8
- 238000004140 cleaning Methods 0.000 claims description 7
- 238000000227 grinding Methods 0.000 claims description 2
- 229910052739 hydrogen Inorganic materials 0.000 abstract description 21
- 239000011941 photocatalyst Substances 0.000 abstract description 19
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 abstract description 18
- 239000001257 hydrogen Substances 0.000 abstract description 18
- 238000000034 method Methods 0.000 abstract description 9
- 230000001276 controlling effect Effects 0.000 abstract 1
- 239000003054 catalyst Substances 0.000 description 18
- 239000013078 crystal Substances 0.000 description 12
- 238000001035 drying Methods 0.000 description 10
- 230000001699 photocatalysis Effects 0.000 description 10
- 238000004519 manufacturing process Methods 0.000 description 7
- 239000000463 material Substances 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
- 238000005516 engineering process Methods 0.000 description 5
- 230000000630 rising effect Effects 0.000 description 5
- 229910052757 nitrogen Inorganic materials 0.000 description 4
- 241000282414 Homo sapiens Species 0.000 description 3
- 230000005540 biological transmission Effects 0.000 description 3
- 229910052799 carbon Inorganic materials 0.000 description 3
- 230000008859 change Effects 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 3
- 238000009826 distribution Methods 0.000 description 3
- 239000000203 mixture Substances 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
- 239000000969 carrier Substances 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 239000002803 fossil fuel Substances 0.000 description 2
- 238000005286 illumination Methods 0.000 description 2
- 231100000252 nontoxic Toxicity 0.000 description 2
- 230000003000 nontoxic effect Effects 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
- 238000000862 absorption spectrum Methods 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000001311 chemical methods and process Methods 0.000 description 1
- 230000003749 cleanliness Effects 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000007812 deficiency Effects 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 230000006872 improvement Effects 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
- 238000007146 photocatalysis Methods 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 239000002243 precursor Substances 0.000 description 1
- 125000002924 primary amino group Chemical group [H]N([H])* 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000006798 recombination Effects 0.000 description 1
- 238000005215 recombination Methods 0.000 description 1
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- 239000007787 solid Substances 0.000 description 1
- 230000001052 transient effect Effects 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
Classifications
-
- 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—
-
- 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
-
- 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
-
- 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
Abstract
The invention relates to a photocatalyst, in particular to a preparation method for regulating and controlling the crystallinity of g-C3N 4. Successful alignment of g-C using simple template method 3 N 4 The crystallinity of (2) is regulated and controlled to prepare g-C with proper crystallinity 3 N 4 Photocatalyst (CMCCN-5), and the prepared g-C with optimized crystallinity 3 N 4 The photocatalyst is applied to prepare 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 prepares the hydrogen for g-C by using a simple template method 3 N 4 The crystallinity of (2) is regulated and controlled to prepare g-C with proper crystallinity 3 N 4 Photocatalyst (CMCCN-5), and the prepared g-C with optimized crystallinity 3 N 4 The photocatalyst is applied to prepare hydrogen by decomposing water under visible light.
Background
With the massive consumption of fossil fuels and the continued development of modern industry, energy deficiency has become a major problem in restricting the development of human socioeconomic performance in the 21 st century. In addition, the problem of massive pollution from fossil fuel combustion has led to heavy disasters for human beings. Therefore, from the long-term and sustainable development of human society, there is an urgent need to develop an environment-friendly and renewable technology that can be used for green production of energy and solving environmental problems. Among the numerous strategies proposed, photocatalytic technology, which has the advantages of economy, cleanliness, safety, sustainability, etc., is considered as an effective approach to solving energy shortages and environmental problems. 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 non-toxic and harmless substances through an environment-friendly chemical process.
In recent years, nonmetallic polymers-g-C 3 N 4 The material is cheap, the preparation is simple, the material is driven by visible light (the band gap is about 2.7 eV), the material is nontoxic, and the material has a unique electronic energy band structure, excellent physical and chemical stability and other advantages, so that the material is widely focused by the scientific research field. Despite the advantages mentioned above, for pure, unmodified g-C 3 N 4 The photocatalyst has the advantages that the fact that the separation efficiency of photo-generated carriers in the photocatalytic reaction is low still cannot be overcome, the low charge separation efficiency directly leads to the low photocatalytic performance, and the practical application standard cannot be met. The main cause of these defects is the bulk phase g-C 3 N 4 Is amorphous, and a large number of carrier recombination centers exist on the surface, so that the photocatalytic activity of the amorphous material is low. A large number of researchers have successfully prepared g-C with high crystallinity 3 N 4 The photocatalyst has excellent photo-generated carrier separation capability. However, g-C having high crystallinity 3 N 4 The catalyst eliminates a large number of non-condensed amino groups, so that the catalyst lacks reactive sites and cannot efficiently utilize photo-generated carriers. Thus, there is a need for g-C 3 N 4 The crystallinity of (2) is optimized, and the high crystallinity g-C is further improved by constructing more reactive sites 3 N 4 Is used for the photocatalytic performance of the catalyst.
Disclosure of Invention
The invention aims to provide a graphite phase carbon nitride (CMCCN-x) photocatalyst with optimized crystallinity and a preparation method thereof, and examine the application of the photocatalyst in preparing hydrogen by decomposing water under visible light, and the photocatalyst is prepared by reacting g-C 3 N 4 The crystallinity is optimized, more reactive sites are constructed while the high-efficiency carrier separation capability is maintained, so that the prepared CMCCN-5 photocatalyst has higher light utilization rate and shows excellent hydrogen preparation performance of fuel by decomposing water under visible light.
The present invention achieves the above object by the following means.
Regulation and control g-C 3 N 4 The preparation method of the crystallinity is characterized by comprising the following steps:
after cyanuric acid, melamine, potassium chloride and absolute ethyl alcohol are ground uniformly, placing the ground cyanuric acid, melamine, potassium chloride and absolute ethyl alcohol in a baking oven for drying, placing the dried cyanuric acid, the melamine, the potassium chloride and the absolute ethyl alcohol in a porcelain boat, placing the porcelain boat in a tubular furnace for calcining 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 baking oven.
Further, the mass ratio of cyanuric acid, melamine and potassium chloride is as follows: 1-5:0.1-3:0.5-5 g of potassium chloride and absolute ethyl alcohol: 1-3mL.
Further, the calcination temperature is 500-650 ℃, and the temperature rising rate is 1-10 ℃/min.
Preferably, the mass ratio of cyanuric acid, melamine and potassium chloride is 2.5:0.5:2, the ratio of potassium chloride to absolute ethanol is 2g:1mL, the calcination temperature is 550 ℃, the temperature rising rate is 5 ℃/min, and the calcination time is 4h.
By contrast, the phase g-C 3 N 4 The preparation method of (PCN) is as follows
And (3) uniformly grinding melamine and absolute ethyl alcohol, placing the mixture into a baking oven for baking, placing the baking oven into a porcelain boat, and then placing the porcelain boat into a tube furnace for calcining for 1-8h under argon atmosphere.
Further, the mass of melamine is 1-8g, and the volume of absolute ethyl alcohol is 1-3mL.
Further, the calcining temperature of the tube 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 temperature rising rate is 5 ℃/min, and the calcination time is 4h.
KCl template method for preparing bulk phase g-C 3 N 4 The method of (PCNS) is as follows:
after being uniformly ground, melamine, potassium chloride and absolute ethyl alcohol are put into a baking oven for baking, then are put into a porcelain boat, are put into a tube furnace for calcination for 1-8 hours under argon atmosphere, are then cleaned by deionized water and absolute ethyl alcohol, and are baked by the baking oven.
Further, the mass ratio of melamine to potassium chloride is 1-8:0.5-5 g of potassium chloride and absolute ethyl alcohol: 1-3mL.
Further, the calcining temperature of the tube 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 ethanol is 2g:1mL, the calcination temperature is 550 ℃, the temperature rising rate is 5 ℃/min, and the calcination time is 4h.
High crystallinity g-C 3 N 4 The preparation method of (CCN) comprises the following steps:
after cyanuric acid, potassium chloride and absolute ethyl alcohol are ground uniformly, the ground cyanuric acid, the potassium chloride and the absolute ethyl alcohol are placed in a baking oven for drying, then the dried cyanuric acid, the potassium chloride and the absolute ethyl alcohol are placed in a porcelain boat, then the porcelain boat is placed in a tubular furnace for calcining for 1-8h under argon atmosphere, and then deionized water and the absolute ethyl alcohol are used for cleaning, and the porcelain boat is baked in the baking oven.
Further, the mass ratio of cyanuric acid to potassium chloride is 1-8:0.5-5 g of potassium chloride and absolute ethyl alcohol: 1-3mL.
Further, the calcining temperature of the tube 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 ethanol is 2g:1mL, the calcination temperature is 550 ℃, the temperature rising rate is 5 ℃/min, and the calcination time is 4h.
The beneficial effects of the invention are that
The invention has the advantages that g-C is optimized simply 3 N 4 And will optimize the crystallinity of g-C 3 N 4 The catalyst has good photocatalytic performance for decomposing water to prepare hydrogen. Compared with the traditional g-C, the CMCCN-5 provided by the invention 3 N 4 The carrier separation is better, the photon utilization efficiency is higher, so that the high-efficiency photocatalytic activity of the prepared photocatalyst is exerted, the method does not cause resource waste, and the method is simple and convenient to operate and low in cost, and is an environment-friendly high-efficiency treatment technology.
Drawings
FIG. 1a is an X-ray diffraction pattern of the prepared catalyst at 2 theta=10° -40 °, from which it can be seen that PCN and PCNS have diffraction peaks at 13 DEG and 27 DEG at 2 theta and amorphous phase g-C 3 N 4 Completely coincide, but the characteristic peak of CMCCN-5 and CCN at about 13 degrees is not seen, and the characteristic peak of (002) crystal face moves from 27 degrees to 28 degrees, which indicates that CMCCN-5 and CCThe crystal structure of N is significantly changed. Further comparing the half-widths of (002) crystal planes of the prepared samples, it was found 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 at 2θ=10° -80 °, and the half-width of the (002) crystal plane of CMCCN-5 is significantly larger than that of CCN, indicating that the method can effectively change g-C 3 N 4 Is a crystal of (a) is a crystal of (b).
Fig. 2a-f are transmission diagrams of the prepared catalyst: fig. 2a is a SAED and projection view of CCN, showing that CCN has a distinct distribution of bright spots. FIGS. 2b-c are high resolution views of CCN transmitted, and obvious 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 plots of CMCCN-5, which show only some locally apparent lattice fringes, most of which are random, indicating a significant decrease in crystallinity. The above proves that the control of the amino content of the raw materials can effectively control the g-C 3 N 4 Is a crystal of (a) is a crystal of (b). FIG. 2g is a distribution diagram of the elements of CMCCN-5, showing that C, N, O, cl and K are uniformly distributed.
FIG. 3a is a steady state fluorescence plot of the prepared catalyst, it can be seen that with g-C 3 N 4 The crystallinity is improved, and the fluorescence intensity is reduced in turn. 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 indicate g-C 3 N 4 The improvement of crystallinity can effectively enhance the carrier separation capability of the catalyst, and also proves that the method can effectively regulate and control g-C 3 N 4 Is a crystal of (a) is a crystal of (b). FIG. 3d is an infrared absorption spectrum of the prepared catalyst, and it can be seen that all samples were at 550cm -1 To 1800cm -1 All show typical g-C 3 N 4 Characteristic absorption peaks. Furthermore, 3100cm -1 at-NH x Shows a significant difference between the characteristic peaks of the (C) and-NH of the highly crystalline samples (CMCCN-5 and CCN) x The content is obviously reduced. This indicates-NH x For g-C 3 N 4 Has a critical influence on the crystal formation. FIG. 3e shows the electron paramagnetic resonance of the prepared sample, which can be seenNo obvious change in formant intensity of the prepared sample indicates that the change of the precursor is relative to g-C 3 N 4 The formation of the internal lone pair of electrons has no obvious effect. 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 that the catalyst is used for g-C 3 N 4 The regulation of the crystal of the light absorption range of the light-emitting diode has no obvious influence.
Table 1 shows the element content 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 content of C, N and H of CMCCN-5 and CCN is obviously reduced compared with that of PCN and PCNS. Further, there was a significant increase in the N and H content of CMCCN-5 over CCN, indicating that more amine groups were generated in CMCCN-5 that were not fully reacted.
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 largest specific surface area value, which indicates that CMCCN-5 can provide more reactive sites and promote the photocatalytic reaction. FIG. 4b is a graph showing the hydrogen production of the prepared catalyst for 5 hours, from which it can be seen that CMCCN-5 has the highest hydrogen production at the same time, indicating that CMCCN-5 has the best performance. FIG. 4c is a graph of the average hydrogen production rate over 5 hours for the hydrogen production reaction of the prepared catalyst, from which it can be seen that CMCCN-5 has the greatest value, indicating that 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 efficiencies of CMCCN-5 at 420nm and 450nm reach 26.9% and 14.0%, respectively, indicating that it can efficiently convert and utilize the absorbed visible light.
Detailed Description
Example 1
Preparation of PCN photocatalyst:
after 5g of melamine and 1mL of absolute ethyl alcohol are ground uniformly, the mixture is put into a baking oven for drying, then is put into a porcelain boat, is put into a tube furnace for argon atmosphere, is heated to 550 ℃ at a heating rate of 5 ℃/min, and is calcined for 4 hours at 550 ℃. And then cleaning with deionized water and absolute ethyl alcohol, and drying by an oven.
Example 2
Preparation of PCNS photocatalyst:
after 3g of melamine, 2g of potassium chloride and 1mL of absolute ethyl alcohol are ground uniformly, the mixture is placed in an oven for drying, then placed in a porcelain boat, placed in a tube furnace under argon atmosphere, heated to 550 ℃ at a heating rate of 5 ℃/min, and calcined for 4 hours at 550 ℃. And then cleaning with deionized water and absolute ethyl alcohol, and drying by an oven.
Example 3
Preparation of CCN photocatalyst:
3g cyanuric acid, 2g potassium chloride and 1mL absolute ethyl alcohol are ground uniformly, then are put into a baking oven for baking, are put into a porcelain boat, are then put into a tube furnace for argon atmosphere, are heated to 550 ℃ at a heating rate of 5 ℃/min, and are calcined for 4 hours at 550 ℃. And then cleaning with deionized water and absolute ethyl alcohol, and drying by an oven.
Example 4
Preparation of CMCCN-5 photocatalyst (invention):
2.5g of cyanuric acid, 0.5g of melamine, 2g of potassium chloride and 1mL of absolute ethyl alcohol are uniformly ground, placed in an oven for drying, placed in a porcelain boat, placed in a tube furnace under argon atmosphere, heated to 550 ℃ at a heating rate of 5 ℃/min, and calcined at 550 ℃ for 4 hours. And then cleaning with deionized water and absolute ethyl alcohol, and drying by an oven.
Example 5
The experimental process of preparing hydrogen by photocatalytic water splitting comprises the following steps: 0.05g of catalyst was weighed and dispersed in 100mL of a solution, wherein the 100mL of solution contained 20% (20 mL) triethanolamine, 3wt% (0.0015 g) Pt. Before illumination, argon is introduced into the reaction vessel, so that air in the reactor is discharged, and the influence of the air on the generation of hydrogen for decomposing water is avoided. And injecting hydrogen generated by the reaction into the gas chromatograph every 1 hour, and finally calculating the hydrogen yield. It can be seen from FIG. 4b that the prepared CMCCN-5 photocatalyst has excellent hydrogen production activity by decomposing water with visible light.
TABLE 1
Claims (3)
1. Regulation and control g-C 3 N 4 Preparation of crystallinity by reacting g-C 3 N 4 The crystallinity of (2) is optimized, and g-C is further improved by constructing more reactive sites 3 N 4 Uniformly grinding cyanuric acid, melamine, potassium chloride and absolute ethyl alcohol, placing the ground cyanuric acid, melamine, potassium chloride and absolute ethyl alcohol in a baking oven for baking, placing the baked cyanuric acid, potassium chloride and absolute ethyl alcohol in a porcelain boat, placing the porcelain boat in a tubular furnace for calcining 1-8h in an argon atmosphere, cleaning the porcelain boat with deionized water and absolute ethyl alcohol, and baking the porcelain boat in the baking oven; the mass ratio of cyanuric acid, melamine and potassium chloride is 2.5:0.5:2, the ratio of potassium chloride to absolute ethanol is 2g:1 mL.
2. A regulatory g-C of claim 1 3 N 4 The 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.
3. A regulatory g-C of claim 2 3 N 4 The 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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| CN113967481B (en) * | 2021-11-25 | 2024-02-27 | 江苏科技大学 | Spherical MoP-HCCN-like composite photocatalyst and preparation method and application thereof |
| 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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