CN113244943B - Composite graphite phase carbon nitride material and preparation method and application thereof - Google Patents
Composite graphite phase carbon nitride material and preparation method and application thereof Download PDFInfo
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- JMANVNJQNLATNU-UHFFFAOYSA-N oxalonitrile Chemical compound N#CC#N JMANVNJQNLATNU-UHFFFAOYSA-N 0.000 title claims abstract description 100
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- ZPWVASYFFYYZEW-UHFFFAOYSA-L dipotassium hydrogen phosphate Chemical group [K+].[K+].OP([O-])([O-])=O ZPWVASYFFYYZEW-UHFFFAOYSA-L 0.000 claims description 15
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- 239000011574 phosphorus Substances 0.000 claims description 9
- 239000011591 potassium Substances 0.000 claims description 9
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- 229910052573 porcelain Inorganic materials 0.000 description 8
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 6
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- -1 carbon nitrides Chemical class 0.000 description 3
- 239000008367 deionised water Substances 0.000 description 3
- 229910021641 deionized water Inorganic materials 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 238000002441 X-ray diffraction Methods 0.000 description 2
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- APUPEJJSWDHEBO-UHFFFAOYSA-P ammonium molybdate Chemical compound [NH4+].[NH4+].[O-][Mo]([O-])(=O)=O APUPEJJSWDHEBO-UHFFFAOYSA-P 0.000 description 1
- 229940010552 ammonium molybdate Drugs 0.000 description 1
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- 239000011609 ammonium molybdate Substances 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- PYKYMHQGRFAEBM-UHFFFAOYSA-N anthraquinone Natural products CCC(=O)c1c(O)c2C(=O)C3C(C=CC=C3O)C(=O)c2cc1CC(=O)OC PYKYMHQGRFAEBM-UHFFFAOYSA-N 0.000 description 1
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- MNNHAPBLZZVQHP-UHFFFAOYSA-N diammonium hydrogen phosphate Chemical compound [NH4+].[NH4+].OP([O-])([O-])=O MNNHAPBLZZVQHP-UHFFFAOYSA-N 0.000 description 1
- 229910000388 diammonium phosphate Inorganic materials 0.000 description 1
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- 230000001699 photocatalysis Effects 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
-
- 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
- C01B15/00—Peroxides; Peroxyhydrates; Peroxyacids or salts thereof; Superoxides; Ozonides
- C01B15/01—Hydrogen peroxide
- C01B15/027—Preparation from water
-
- 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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- Chemical & Material Sciences (AREA)
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- Engineering & Computer Science (AREA)
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- Chemical Kinetics & Catalysis (AREA)
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Abstract
The invention belongs to the technical field of nano material preparation, and particularly relates to a composite graphite phase carbon nitride material as well as a preparation method and application thereof. By usingK, P, O and S are doped into the graphite phase carbon nitride structure by the thermal polymerization method, and the doping of the elements not only reduces the band gap width of the graphite phase carbon nitride, but also effectively increases the utilization rate of visible light and accelerates the transmission rate of photon-generated carriers. The visible light catalyst with higher catalytic activity is screened out, and H is promoted 2 O 2 Is efficiently generated.
Description
Technical Field
The invention belongs to the technical field of nano material preparation, and particularly relates to a composite graphite phase carbon nitride material as well as a preparation method and application thereof.
Background
The information in this background section is only for enhancement of understanding of the general background of the invention and is not necessarily to be construed as an admission or any form of suggestion that this information forms the prior art that is already known to a person of ordinary skill in the art.
Hydrogen peroxide is a strong oxidant commonly used in the industry, and has been widely used in organic synthesis, environmental remediation, disinfection, liquid propellants, and the like because the reaction product only generates water and oxygen. Currently, H is commercially produced 2 O 2 The anthraquinone process results in great power consumption and environmental pollution caused by the production of pollutant. Therefore, an inexpensive production H was developed 2 O 2 The green process of (2) is in great demand.
Graphite phase carbon nitride (g-C) 3 N 4 ) Is a non-metallic inorganic semiconductor that is of great interest because of its high energy structure suitable for water decomposition, oxygen Reduction Reaction (ORR) and organic contaminant degradation. Although the photocatalyst has been used for producing H 2 O 2 However, a graphite phaseThe rapid recombination of photogenerated electron-hole pairs in carbon nitride results in lower H 2 O 2 The yield limits the practical application of the graphite phase carbon nitride, and the quantum efficiency and the photocatalytic performance of the graphite phase carbon nitride must be further improved.
Some prior art techniques dope graphite phase carbon nitride materials with elements to raise H 2 O 2 Production efficiency, but the inventor researches and discovers that the elements catalyze the preparation of H by the graphite phase carbon nitride material 2 O 2 Has limited effect on improving and catalytically produces H with prolonged catalytic time 2 O 2 The effect of (A) is reduced to some extent, H 2 O 2 The rate of yield increase decreases.
Disclosure of Invention
In order to further improve the catalytic production of H by the graphite phase carbon nitride material 2 O 2 The invention provides a composite graphite phase carbon nitride material and a preparation method and application thereof, wherein K, P, O and S are doped into a graphite phase carbon nitride structure by utilizing a thermal polymerization method, and the doping of elements not only reduces the band gap width of the graphite phase carbon nitride, but also effectively increases the utilization rate of visible light and accelerates the transmission rate of photon-generated carriers. Screening out visible light catalyst with high catalytic activity and promoting H 2 O 2 Efficient generation of (1).
Specifically, the invention is realized by the following technical scheme:
in a first aspect of the invention, a composite graphite phase carbon nitride material is provided, wherein the composite graphite phase carbon nitride material loads K, P, O and S elements.
In a second aspect of the present invention, a method for preparing a composite graphite-phase carbon nitride material is provided, which comprises mixing a potassium source, a phosphorus source, a sulfur source and urea, and sintering.
In a third aspect of the invention, a composite graphite phase carbon nitride material is provided for synthesizing H 2 O 2 The use of (1).
In a fourth aspect of the invention, there is provided a method of producing H 2 O 2 A synthesis catalyst comprising the composite graphitic phase nitrogen according to claim 1A carbonized material.
One or more embodiments of the present invention have the following advantageous effects:
1) By doping K, P, O and S into the graphite-phase carbon nitride structure, the doping of the K, P, O and S elements not only reduces the band gap width of the graphite-phase carbon nitride, but also effectively increases the utilization rate of visible light and accelerates the transmission rate of photon-generated carriers. Screening out visible light catalyst with high catalytic activity and promoting H 2 O 2 Efficient generation of (1).
2) The research of the invention discovers that the traditional visible light catalyst is used for catalyzing and producing H 2 O 2 In this case, the catalytic effect decreases as the catalyst life increases. The interaction of K, P, O and S elements is helpful to improve the catalytic production of H from the composite graphite phase carbon nitride material 2 O 2 Stability in time.
Drawings
The accompanying drawings, which are incorporated in and constitute a part of this specification, are included to provide a further understanding of the invention, and are incorporated in and constitute a part of this specification, illustrate exemplary embodiments of the invention and together with the description serve to explain the invention and not to limit the invention. Embodiments of the invention are described in detail below with reference to the attached drawing figures, wherein:
FIG. 1 is a scanning electron microscope image of graphite-phase carbon nitride prepared in Experimental example 1 of the present invention;
FIG. 2 shows the K, P, O, S modified graphite-phase carbon nitride (K, P, O, S-g-C) prepared in Experimental example 2 3 N 4 ) Scanning an electron microscope picture;
FIG. 3 is a graph showing graphite-phase carbon nitrides (g-C) prepared in the experimental examples of the present invention and in comparative examples 1 to 4 3 N 4 ) And the proportions of K, P, O-graphite phase carbon nitride (K, P, O-g-C) 3 N 4 ) And K, P, O, S-graphite phase carbon nitride (K, P, O, S-g-C) 3 N 4 ) An XRD pattern of (a);
FIG. 4 is a graph showing graphite-phase carbon nitrides (g-C) prepared in the experimental examples of the present invention and in comparative examples 1 to 4 3 N 4 ) And the ratio of K, P, O-graphite phase carbon nitride (K, P, O-g-C) 3 N 4 ) And K, P, O, S-graphite phase carbon nitride (K, P, O, S-g-C) 3 N 4 ) H of (A) to (B) 2 O 2 A photosynthesized curve;
FIG. 5 shows graphite-phase carbon nitrides (g-C) prepared in the experimental examples of the present invention and comparative examples 3,5 and 7 3 N 4 ) K, P, O-graphite phase carbon nitride (K, P, O-g-C) 3 N 4 ) Single element doped graphite phase carbon nitride and K, P, O, S-graphite phase carbon nitride (K, P, O, S-g-C) 3 N 4 ) H of (A) to (B) 2 O 2 And (4) synthesizing the curve by light.
Detailed Description
The invention will be further illustrated with reference to the following specific examples. It should be understood that these examples are for illustrative purposes only and are not intended to limit the scope of the present invention. The experimental procedures, in which specific conditions are not noted in the following examples, are generally carried out according to conventional conditions or according to conditions recommended by the manufacturers.
It is noted that the terminology used herein is for the purpose of describing particular embodiments only and is not intended to be limiting of example embodiments according to the present disclosure. As used herein, the singular forms "a", "an" and "the" are intended to include the plural forms as well, and it should be understood that when the terms "comprises" and/or "comprising" are used in this specification, they specify the presence of stated features, steps, operations, devices, components, and/or combinations thereof, unless the context clearly indicates otherwise.
In order to further improve the catalytic production of H by the graphite phase carbon nitride material 2 O 2 The invention provides a composite graphite phase carbon nitride material and a preparation method and application thereof, wherein K, P, O and S are doped into a graphite phase carbon nitride structure by utilizing a thermal polymerization method, and the doping of elements not only reduces the band gap width of the graphite phase carbon nitride, but also effectively increases the utilization rate of visible light and accelerates the transmission rate of photon-generated carriers. The visible light catalyst with higher catalytic activity is screened out, and H is promoted 2 O 2 Efficient generation of (1).
Specifically, the invention is realized by the following technical scheme:
in a first aspect of the invention, a composite graphite phase carbon nitride material is provided, wherein the composite graphite phase carbon nitride material loads K, P, O and S elements.
Although the prior art discloses the doping of K or P elements into graphite phase carbon nitride materials for improving the catalytic production of H from graphite phase carbon nitride materials 2 O 2 However, the inventor researches and discovers that the catalysts have the defects of poor catalytic effect and insufficient stability, so that the S element is introduced into the invention to be cooperated with K, P and O to promote the composite graphite phase carbon nitride material to catalytically produce H 2 O 2 Efficiency and stability of the process. The deep analysis principle shows that the doping of the K, P, O and S elements not only reduces the band gap width of the graphite phase carbon nitride, but also effectively increases the utilization rate of visible light and accelerates the transmission rate of photon-generated carriers. The visible light catalyst with higher catalytic activity is screened out, and H is promoted 2 O 2 Is efficiently generated.
In a second aspect of the present invention, a method for preparing a composite graphite-phase carbon nitride material is provided, which comprises mixing a potassium source, a phosphorus source, a sulfur source and urea, and sintering.
The raw material source influences the element load uniformity and the interaction among elements, and experiments show that when the potassium source is selected from dipotassium hydrogen phosphate, the phosphorus source is selected from dipotassium hydrogen phosphate, and the sulfur source is selected from thiourea, the prepared composite graphite phase carbon nitride material is used for producing H under the catalysis of 2 O 2 The efficiency of (2) is higher.
Further research shows that K and P have better synergistic effect when the potassium source and the phosphorus source are selected from substances containing potassium and phosphorus at the same time, and dipotassium hydrogen phosphate is preferred, and the catalytic performance of the composite graphite phase carbon nitride material prepared by using the dipotassium hydrogen phosphate is better than that of the composite graphite phase carbon nitride material prepared by using different K sources and P sources.
The loading capacity of elements in the composite graphite phase carbon nitride material is determined by the raw material proportion, and when the mass ratio of dipotassium hydrogen phosphate, the sulfur source and the urea is as follows: 0.02-2.28, the molar ratio of K, P, O and S elements is 0.02-2:0.01-1:15-28:11-18, under the condition of the element proportion, the four elements can obviously promote the composite graphite phase carbon nitride material to catalytically produce H 2 O 2 The efficiency of (c).
The inventor is oversizeThe amount research shows that when the mass ratio of the dipotassium hydrogen phosphate, the sulfur source and the urea is as follows: 0.68 2 O 2 The yield still increased. The problem of catalytic stop occurs after the traditional catalyst is used for 180min, H 2 O 2 The yield is not increased any more.
Experiments also find that when the mass ratio of the sulfur source to the urea is 1 2 O 2 Still have a high level of efficiency.
In the preparation process, the sintering temperature and time influence the morphology and element distribution of the composite graphite phase carbon nitride material, and when the sintering temperature is 500-600 ℃, and the sintering temperature is kept for 2-5h, the graphite phase carbon nitride has a complete lamellar structure, which is beneficial to the uniform distribution of K, P, O and S elements.
The temperature rise rate in the sintering process affects the uniformity of elements, is too fast, elements are not distributed in the graphite phase carbon nitride lamellar structure in time, and is too slow, so that the generation of the graphite phase carbon nitride lamellar structure is not facilitated, and therefore, in one or more embodiments of the invention, the temperature rise rate in the sintering process is 5-10 ℃/min.
In one or more embodiments of the invention, the temperature rise rate is 5 ℃/min, the temperature rises to 550 ℃, and the composite graphite phase carbon nitride material prepared has good catalytic stability when the temperature is maintained for 3 hours.
In a third aspect of the invention, a composite graphite phase carbon nitride material is provided for synthesizing H 2 O 2 The use of (1).
Preferably, H is synthesized under visible light 2 O 2 The use of (1).
In a fourth aspect of the invention, there is provided a method of producing H 2 O 2 A synthesis catalyst comprising the composite graphite phase carbon nitride material of claim 1.
The present invention is described in further detail below with reference to specific examples, which are intended to be illustrative of the invention and not limiting.
In the following method of the invention, the equipment and reagents used are as follows:
TABLE 1 instrumentation
TABLE 2 major reagents
Experimental example 1 graphite phase carbon nitride powder (g-C) 3 N 4 ) Preparation of (2)
50g of urea was weighed into a porcelain crucible with a lid, placed in a forced air drying oven until the urea was completely dried, and then transferred to a muffle furnace. Raising the temperature to 550 ℃ at the heating rate of 5 ℃/min, and keeping the temperature for 3 hours to finally obtain the faint yellow graphite-phase carbon nitride powder.
Experimental example 2K, P, O, S-graphite phase carbon nitride (K, P, O, S-g-C) 3 N 4 ) Preparation of the powder
0.68g of dipotassium hydrogen phosphate, 11.42g of thiourea and 11.42g of urea are weighed respectively, uniformly mixed, ground, placed into a porcelain crucible with a cover and transferred into a muffle furnace. Heating to 550 ℃ at a heating rate of 5 ℃/min, and keeping for 3h, so as to finally obtain the graphite-phase carbon nitride powder modified by K, P, O and S with a mass ratio of 5% (molar ratio K: P: O: S = 0.7.
Comparative example 1
22.84mg of dipotassium hydrogenphosphate and 22.84g of urea were weighed, mixed, ground, placed in a porcelain crucible with a lid, and transferred to a muffle furnace. Heating to 550 ℃ at a heating rate of 5 ℃/min, and keeping for 3 hours to obtain the K, P, O modified graphite phase carbon nitride (K, P, O-g-C) with the mass ratio of 0.1 percent 3 N 4 ) The sum of the mass of the powder, K, P and O elements is 0.1 percent of the composite catalyst.
Comparative example 2
228.44mg of dipotassium hydrogenphosphate and 22.84g of urea were weighed, mixed, ground, placed in a porcelain crucible with a lid, and transferred to a muffle furnace. Heating to 550 ℃ at the heating rate of 5 ℃/min, and keeping for 3 hours to obtain the K, P, O modified graphite phase carbon nitride (K, P, O-g-C) with the mass ratio of 1 percent 3 N 4 ) The sum of the mass of the powder, K, P and O elements is 1 percent of the composite catalyst.
Comparative example 3
1.14g of dipotassium hydrogenphosphate and 22.84g of urea were weighed, mixed, ground, placed in a porcelain crucible with a lid, and transferred into a muffle furnace. Heating to 550 ℃ at the heating rate of 5 ℃/min, and keeping for 3 hours to prepare the K, P, O modified graphite phase carbon nitride (K, P, O-g-C) with the mass ratio of 5 percent 3 N 4 ) The sum of the mass of the powder, K, P and O elements is 5 percent of the composite catalyst.
Comparative example 4
2.28g of dipotassium hydrogenphosphate and 22.84g of urea were weighed, mixed, ground, placed in a porcelain crucible with a lid, and transferred to a muffle furnace. Heating to 550 ℃ at the heating rate of 5 ℃/min, and keeping for 3 hours to obtain the K, P, O modified graphite phase carbon nitride (K, P, O-g-C) with the mass ratio of 10 percent 3 N 4 ) The sum of the mass of the powder, K, P and O elements is 10 percent of the composite catalyst.
Comparative example 5
11.42g of thiourea and 11.42g of urea were weighed, mixed uniformly, ground, placed in a porcelain crucible with a lid, and transferred into a muffle furnace. Heating to 550 deg.C at a rate of 5 deg.C/min, and maintaining for 3 hr to obtain S-modified graphite phase carbon nitride powder, i.e. S-graphite phase carbon nitride (S-g-C) 3 N 4 )。
Comparative example 6
12g of urea and 0.4g of KNO are weighed 3 Dissolved in 60mL of deionized water, stirred and water-bath dried at 70 ℃. The mixture was ground, placed in a porcelain crucible with a lid, and transferred to a muffle furnace. The temperature is raised to 550 ℃ at a heating rate of 5 ℃/min and is kept for 3 hours. Subsequently, the product was ground to a powder and heated at 350 ℃ toCalcining at 10 deg.C in air for 3 hr to obtain K-modified graphite-phase carbon nitride powder, i.e. K-graphite-phase carbon nitride (K-g-C) 3 N 4 )。
Comparative example 7
Weighing 10g of urea, 0.2g of diammonium hydrogen phosphate and 50mL of deionized water, uniformly mixing, transferring into a crucible, drying at 65 ℃ for 12 hours, grinding, putting into a ceramic crucible with a cover, and transferring into a muffle furnace. Heating to 500 deg.C at a rate of 5 deg.C/min, and maintaining for 3 hr to obtain P-modified graphite phase carbon nitride powder, i.e. P-graphite phase carbon nitride (P-g-C) 3 N 4 )。
H 2 O 2 Catalytic experiment
In 135mL of deionized water and 15mL of an isopropyl alcohol mixed solvent (isopropyl alcohol volume fraction: 10 vol%), dilute hydrochloric acid was slowly added dropwise to pH =3.0-4.0, followed by addition of 0.15g of the photocatalyst prepared in the above examples and comparative examples, and passing high purity oxygen for 30min to bring the solution to an oxygen saturation state, and irradiation was performed with a 300W (λ >420 nm) xenon lamp for 150min. After the reaction solution was extracted, the reaction solution was placed in a colorimetric tube containing a mixed solution of 8mL 1M KI and 0.2mL 0.01M ammonium molybdate, and the absorbance value of the reaction solution at the wavelength of 352nm was measured by an ultraviolet-visible spectrophotometer.
As shown in fig. 1, the graphite-phase carbon nitride prepared in experimental example 1 exhibited a two-dimensional sheet-like and layered porous structure. The K, P, O, S-graphite phase carbon nitride (figure 2) prepared in the experimental example 2 can observe that the K, P, O, S-graphite phase carbon nitride still presents a stacked layered structure, and is more obvious, and the structure is beneficial to the catalyst to adsorb more reaction substances and improve the reaction activity.
FIG. 3 is XRD patterns of experimental examples and comparative examples 1 to 4. After three elements of K, P and O are doped into the graphite phase carbon nitride framework structure in situ, K is added 2 HPO 4 The increase in the content shifts the (002) plane of the graphite phase carbon nitride slightly to a smaller angle because the S atom radius is larger than that of the N atom in the graphite phase carbon nitride after the S is substituted for the N atom, and thus the presence of the S atom can be confirmed.
FIG. 4 is a drawing showingSynthesis of H under visible light for Experimental examples and comparative examples 1 to 4 2 O 2 An efficiency map. The production of all catalysts increased with time. The yield of pure graphite phase carbon nitride under the above test conditions was very low, while the yield of hydrogen peroxide after doping with the impurity elements was gradually increased, with the highest yield of K, P, O, S-graphite phase carbon nitride.
FIG. 5 shows the synthesis of H under visible light for the experimental example and comparative examples 3,5 to 7 2 O 2 And (4) an efficiency map. The production of all catalysts increased with time. Wherein H of K, P, O, S-graphite phase carbon nitride 2 O 2 The yield is the highest and is higher than that of graphite phase carbon nitride doped with single element and pure graphite phase carbon nitride. And over prolonged catalytic time, H of K, P, O, S-graphite phase carbon nitride 2 O 2 The yield is still in an increasing trend, which shows that the K, P, O, S-graphite phase carbon nitride catalyst has a continuous catalytic effect, and the single-element graphite phase carbon nitride and simple graphite phase carbon nitride, K, P, O-graphite phase carbon nitride catalyst has a continuous catalytic effect which is not as good as that of the K, P, O, S-graphite phase carbon nitride catalyst.
Although the present invention has been described in detail with reference to the foregoing embodiments, it will be apparent to those skilled in the art that changes may be made in the embodiments and/or equivalents thereof without departing from the spirit and scope of the invention. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (8)
1. A preparation method of a composite graphite phase carbon nitride material is characterized by comprising the steps of mixing a potassium source, a phosphorus source, a sulfur source and urea, and sintering to obtain the composite graphite phase carbon nitride material;
the potassium source is selected from dipotassium hydrogen phosphate, the phosphorus source is selected from dipotassium hydrogen phosphate, and the sulfur source is selected from thiourea;
the mass ratio of the sulfur source to the urea is 1;
the mass ratio of the dipotassium hydrogen phosphate to the sulfur source to the urea is as follows: 0.68:11.42: 11.42.
2. The method for producing a composite graphite phase carbon nitride material according to claim 1, wherein the composite graphite phase carbon nitride material is loaded with K, P, O, and S elements.
3. The method of producing the composite graphite phase carbon nitride material according to claim 1, wherein the potassium source and the phosphorus source are selected from the group consisting of potassium and phosphorus, and dipotassium hydrogen phosphate.
4. The method of preparing a composite graphite phase carbon nitride material according to claim 1, wherein the sintering temperature is 500 to 600 ℃ and is maintained for 2 to 5 hours.
5. The method of preparing a composite graphite phase carbon nitride material according to claim 1, wherein the temperature rise rate during the sintering process is 5 to 10 ℃/min.
6. The method for preparing a composite graphite-phase carbon nitride material according to claim 1, wherein the temperature is raised to 550 ℃ at a rate of 5 ℃/min for 3 hours.
7. Synthesis of H from composite graphite phase carbon nitride material prepared by the method of any one of claims 1 to 6 2 O 2 Characterized by synthesizing H under visible light 2 O 2 The use of (1).
8. H 2 O 2 A synthetic catalyst comprising the composite graphite phase carbon nitride material produced by the method of any one of claims 1 to 6.
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