CN112371160A - Preparation method and use method of high-crystallization wide-absorption carbon nitride photocatalytic material - Google Patents
Preparation method and use method of high-crystallization wide-absorption carbon nitride photocatalytic 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 65
- 239000000463 material Substances 0.000 title claims abstract description 59
- 230000001699 photocatalysis Effects 0.000 title claims abstract description 49
- 238000010521 absorption reaction Methods 0.000 title claims abstract description 36
- 238000000034 method Methods 0.000 title claims abstract description 20
- 238000002425 crystallisation Methods 0.000 title claims abstract description 18
- 238000002360 preparation method Methods 0.000 title claims abstract description 17
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims abstract description 62
- 239000004202 carbamide Substances 0.000 claims abstract description 62
- 238000010438 heat treatment Methods 0.000 claims abstract description 48
- 238000003825 pressing Methods 0.000 claims abstract description 23
- 238000001816 cooling Methods 0.000 claims abstract description 12
- 239000000843 powder Substances 0.000 claims abstract description 12
- 238000000465 moulding Methods 0.000 claims abstract description 3
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 247
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 20
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 13
- 239000001257 hydrogen Substances 0.000 claims description 13
- 229910052739 hydrogen Inorganic materials 0.000 claims description 13
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 12
- 238000000354 decomposition reaction Methods 0.000 claims description 12
- 238000004519 manufacturing process Methods 0.000 claims description 12
- QPLDLSVMHZLSFG-UHFFFAOYSA-N Copper oxide Chemical compound [Cu]=O QPLDLSVMHZLSFG-UHFFFAOYSA-N 0.000 claims description 11
- 239000005751 Copper oxide Substances 0.000 claims description 11
- 229910000431 copper oxide Inorganic materials 0.000 claims description 11
- 238000006303 photolysis reaction Methods 0.000 claims description 10
- 230000015843 photosynthesis, light reaction Effects 0.000 claims description 10
- GSEJCLTVZPLZKY-UHFFFAOYSA-N Triethanolamine Chemical compound OCCN(CCO)CCO GSEJCLTVZPLZKY-UHFFFAOYSA-N 0.000 claims description 7
- 229910052786 argon Inorganic materials 0.000 claims description 6
- 239000007864 aqueous solution Substances 0.000 claims description 5
- 238000006243 chemical reaction Methods 0.000 claims description 4
- 239000002253 acid Substances 0.000 claims description 3
- 239000003795 chemical substances by application Substances 0.000 claims description 3
- 238000007789 sealing Methods 0.000 claims description 3
- 229910052724 xenon Inorganic materials 0.000 claims description 3
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 claims description 3
- 238000010924 continuous production Methods 0.000 abstract description 2
- 229910052751 metal Inorganic materials 0.000 abstract description 2
- 239000002184 metal Substances 0.000 abstract description 2
- 231100000956 nontoxicity Toxicity 0.000 abstract description 2
- 239000002994 raw material Substances 0.000 abstract description 2
- 239000000126 substance Substances 0.000 abstract description 2
- 230000000052 comparative effect Effects 0.000 description 5
- 230000031700 light absorption Effects 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 230000005284 excitation Effects 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 229910052755 nonmetal Inorganic materials 0.000 description 2
- 239000004065 semiconductor Substances 0.000 description 2
- 238000004659 sterilization and disinfection Methods 0.000 description 2
- 238000003917 TEM image Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
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- 238000006731 degradation reaction Methods 0.000 description 1
- 239000005431 greenhouse gas Substances 0.000 description 1
- 230000001678 irradiating effect Effects 0.000 description 1
- 230000004298 light response Effects 0.000 description 1
- 231100000252 nontoxic Toxicity 0.000 description 1
- 230000003000 nontoxic effect Effects 0.000 description 1
- 230000003287 optical effect Effects 0.000 description 1
- 229920000620 organic polymer Polymers 0.000 description 1
- 239000002957 persistent organic pollutant Substances 0.000 description 1
- 239000011941 photocatalyst Substances 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 238000001878 scanning electron micrograph Methods 0.000 description 1
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- 230000002195 synergetic effect Effects 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 239000004408 titanium dioxide Substances 0.000 description 1
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- 238000005303 weighing Methods 0.000 description 1
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- 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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- B01J35/39—
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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
- C01B21/00—Nitrogen; Compounds thereof
- C01B21/06—Binary compounds of nitrogen with metals, with silicon, or with boron, or with carbon, i.e. nitrides; Compounds of nitrogen with more than one metal, silicon or boron
- C01B21/0605—Binary compounds of nitrogen with carbon
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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
- 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
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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
- C01B2203/02—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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- 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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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2002/00—Crystal-structural characteristics
- C01P2002/01—Crystal-structural characteristics depicted by a TEM-image
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- C01P2002/00—Crystal-structural characteristics
- C01P2002/70—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data
- C01P2002/72—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data by d-values or two theta-values, e.g. as X-ray diagram
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- C01P2004/00—Particle morphology
- C01P2004/01—Particle morphology depicted by an image
- C01P2004/03—Particle morphology depicted by an image obtained by SEM
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- C01—INORGANIC CHEMISTRY
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- C01P2004/04—Particle morphology depicted by an image obtained by TEM, STEM, STM or AFM
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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
Abstract
The invention discloses a preparation method of a high-crystallization wide-absorption carbon nitride photocatalytic material, which comprises the following operation steps: (1) pressing and molding urea in a die by adopting a powder tablet machine to obtain a urea tablet; (2) and (3) heating the urea sheet by adopting 900-1100MHz frequency microwave, and naturally cooling to room temperature to obtain the carbon nitride material. The carbon nitride photocatalytic material prepared by the method has high crystallinity, wide photoresponse range, good chemical stability and thermal stability, no metal, no toxicity, no harm, easily obtained raw materials and low price; the method for preparing the modified carbon nitride material with high crystallinity and wide absorption has simple operation and high repeatability, and can realize industrialized continuous production.
Description
Technical Field
The invention belongs to the technical field of photolysis catalytic reaction, and particularly relates to a preparation method and a use method of a high-crystallization wide-absorption carbon nitride photocatalytic material.
Background
With the rapid development of human society, the demand for energy is increasing day by day, and simultaneously, a large amount of fossil energy is consumed, and a large amount of toxic and greenhouse gases are generated. Causing serious harm to the environment. After titanium dioxide is found to be capable of producing hydrogen by photolysis of water, the semiconductor photocatalytic material is widely applied to the fields of hydrogen production by photolysis of water, carbon dioxide reduction, degradation of organic pollutants, disinfection, sterilization, organic synthesis and the like. However, most of the photocatalytic materials are metallic compounds and have a small sunlight absorption range, so that the environment is polluted, the price cost is increased, and the utilization efficiency of solar energy is reduced. Therefore, the development of visible light response nonmetal photocatalyst is significant.
The graphite phase carbon nitride is a non-metal organic polymer semiconductor material, and has the advantages of no toxicity, no harm, easy preparation, visible light absorption, low price, high stability and the like, so the graphite phase carbon nitride becomes a research hotspot of photocatalytic materials in nearly more than ten years. However, because carbon nitride is a polymer, the crystallinity obtained by the traditional method is low, photogenerated electrons and holes are easy to recombine, and meanwhile, the bandwidth is relatively large (2.7eV), and the carbon nitride can only absorb visible light below 460nm, and the inherent defects finally cause that the photocatalytic efficiency of the carbon nitride material prepared by the traditional method is low.
Disclosure of Invention
Aiming at the problems in the prior art, the invention provides a preparation method and a use method of a high-crystallinity and wide-absorption carbon nitride photocatalytic material, aiming at obtaining a modified carbon nitride material with high crystallinity and a large light absorption range by adopting a strategy of irradiating urea tablets by microwaves, and the final photocatalytic effect is obviously improved by the synergistic effect of the two factors.
The technical scheme adopted for realizing the purpose of the invention is as follows:
a preparation method of a high-crystallization wide-absorption carbon nitride photocatalytic material comprises the following operation steps:
(1) pressing and molding urea in a die by adopting a powder tablet machine to obtain a urea tablet;
(2) and (3) heating the urea sheet by adopting 900-1100MHz frequency microwave, and naturally cooling to room temperature to obtain the carbon nitride material.
Specifically, in the step (1), the pressing pressure is 2-24 MPa.
Specifically, in the step (2), the container during microwave heating of the urea sheet is an alumina crucible, during microwave heating, the urea sheet is firstly placed in the first alumina crucible, then a second alumina crucible with a volume 2 times that of the first alumina crucible is reversely buckled on the first alumina crucible, then the combined crucible is placed in a third alumina crucible with a volume 5 times that of the second alumina crucible, finally, the third alumina crucible is filled with copper oxide, the second alumina crucible is covered, and finally, the three combined crucibles are subjected to microwave heating treatment.
Specifically, in the step (2), the microwave heating treatment time is 25-35 min.
The invention also provides a use method of the high-crystallization wide-absorption carbon nitride photocatalytic material, which comprises the following operation steps:
(1) placing a carbon nitride photocatalytic material in a photocatalytic water decomposition reactor;
(2) adding triethanolamine aqueous solution as a sacrificial agent into a reactor for photocatalytic water decomposition;
(3) adding chloroplatinic acid as a cocatalyst thereto and sealing;
(4) introducing argon into the photocatalytic water decomposition reactor, and removing air in the photocatalytic water decomposition reactor;
(5) and (4) turning on the magnetic stirrer, turning on a light source, and carrying out the photolysis water hydrogen production reaction.
Specifically, in the step (2), the mass fraction of triethanolamine in the triethanolamine aqueous solution is 8-12%.
Specifically, in the step (4), the time for introducing argon is 15-25 min.
Specifically, in the step (5), the light source is a 300W xenon lamp equipped with a filter having a wavelength of 420nm or more.
Specifically, in the step (5), the time for the photolysis water to produce hydrogen is 4 to 6 hours.
According to the technical scheme, the beneficial effects of the invention are as follows:
1) the high-crystallinity and wide-absorption carbon nitride photocatalytic material prepared by the invention has high crystallinity and wide photoresponse range;
2) the high-crystallization wide-absorption carbon nitride photocatalytic material prepared by the invention has good chemical stability and thermal stability;
3) the method for preparing the modified carbon nitride material with high crystallinity and wide absorption has simple operation and high repeatability, and can realize industrialized continuous production;
4. the high-crystallinity and wide-absorption modified carbon nitride material prepared by the invention does not contain metal, is nontoxic and harmless, has easily obtained raw materials and low price;
5. through the test of a model for hydrogen production by water photolysis, the carbon nitride material with high crystallization and wide absorption prepared by the invention has the hydrogen production effect (61.7 mu mol/h) which is nearly 6 times that of the carbon nitride material prepared by the traditional method (10.6 mu mol/h).
Drawings
Fig. 1 is an XRD contrast pattern of the carbon nitride prepared in example 5 and comparative example 1 (002 diffraction peak is significantly enhanced and crystallinity is significantly improved).
FIG. 2 is a graph comparing the UV absorption of the carbon nitride prepared in example 5 and comparative example 1 (new absorption peak at 495nm, broader light absorption).
Fig. 3 is a graph comparing the visible photocurrent (relative intensity of photocurrent is greater and carriers are more easily separated and transported) of the carbon nitride prepared in example 5 and comparative example 1.
Fig. 4 is an SEM image of the carbon nitride prepared in example 5 (wrinkled sheet material, prone to lone pair excitation).
Figure 5 is a TEM image of carbon nitride prepared according to example 5 (wrinkled sheet material, prone to lone pair excitation).
Fig. 6 is a graph of hydrogen production by photolysis of water for a long period of time for carbon nitride prepared in example 5 (illustrating that the carbon nitride material with high crystal and wide absorption prepared by the present invention has strong stability).
FIG. 7 is a graph of the relationship between the wavelength of carbon nitride and the photolytic production of hydrogen (light can be absorbed and the maximum wavelength can reach 535nm) prepared in example 5.
Detailed Description
Embodiments of the present invention will be described in detail below with reference to examples, but it will be understood by those skilled in the art that the following examples are only illustrative of the present invention and should not be construed as limiting the scope of the present invention. The examples, in which specific conditions are not specified, were conducted under conventional conditions or conditions recommended by the manufacturer.
Example 1
A preparation method of a high-crystallization wide-absorption carbon nitride photocatalytic material comprises the following operation steps:
(1) pressing 10g of urea in a die by using a powder tablet press to obtain a urea tablet, wherein the pressing pressure is 2 MPa;
(2) heating urea tablet with 900MHz microwave for 25min, naturally cooling to room temperature to obtain carbon nitride material named CN2-25The container when wherein urea piece microwave heating is the aluminium oxide crucible, during the microwave heating, earlier place the urea piece in first aluminium oxide crucible, then back-off a volume is the second aluminium oxide crucible 2 times of first aluminium oxide crucible on first aluminium oxide crucible, then place the crucible after the combination in the volumetric is the third aluminium oxide crucible 5 times of second aluminium oxide crucible volume, last fill up copper oxide in the third aluminium oxide crucible, cover the second aluminium oxide crucible, carry out microwave heating with the crucible after three combinations at last again and handle.
Example 2
A preparation method of a high-crystallization wide-absorption carbon nitride photocatalytic material comprises the following operation steps:
(1) pressing 10g of urea in a die by using a powder tablet press to obtain a urea tablet, wherein the pressing pressure is 2 MPa;
(2) heating urea tablet with 900MHz microwave for 30min, naturally cooling to room temperature to obtain carbon nitride material named CN2-30The container when wherein urea piece microwave heating is the aluminium oxide crucible, during the microwave heating, earlier place the urea piece in first aluminium oxide crucible, then back-off a volume is the second aluminium oxide crucible 2 times of first aluminium oxide crucible on first aluminium oxide crucible, then place the crucible after the combination in the volumetric is the third aluminium oxide crucible 5 times of second aluminium oxide crucible volume, last fill up copper oxide in the third aluminium oxide crucible, cover the second aluminium oxide crucible, carry out microwave heating with the crucible after three combinations at last again and handle.
Example 3
A preparation method of a high-crystallization wide-absorption carbon nitride photocatalytic material comprises the following operation steps:
(1) pressing 10g of urea in a die by using a powder tablet press to obtain a urea tablet, wherein the pressing pressure is 2 MPa;
(2) heating urea tablet with 950MHz microwave for 35min, naturally cooling to room temperature to obtain carbon nitride material named CN2-35The container when wherein urea piece microwave heating is the aluminium oxide crucible, during the microwave heating, earlier place the urea piece in first aluminium oxide crucible, then back-off a volume is the second aluminium oxide crucible 2 times of first aluminium oxide crucible on first aluminium oxide crucible, then place the crucible after the combination in the volumetric is the third aluminium oxide crucible 5 times of second aluminium oxide crucible volume, last fill up copper oxide in the third aluminium oxide crucible, cover the second aluminium oxide crucible, carry out microwave heating with the crucible after three combinations at last again and handle.
Example 4
A preparation method of a high-crystallization wide-absorption carbon nitride photocatalytic material comprises the following operation steps:
(1) pressing 10g of urea in a die by using a powder tablet press to obtain a urea tablet, wherein the pressing pressure is 8 MPa;
(2) heating urea tablet with 950MHz microwave for 25min, naturally cooling to room temperature to obtain carbon nitride material named CN8-25The container when wherein urea piece microwave heating is the aluminium oxide crucible, during the microwave heating, earlier place the urea piece in first aluminium oxide crucible, then back-off a volume is the second aluminium oxide crucible 2 times of first aluminium oxide crucible on first aluminium oxide crucible, then place the crucible after the combination in the volumetric is the third aluminium oxide crucible 5 times of second aluminium oxide crucible volume, last fill up copper oxide in the third aluminium oxide crucible, cover the second aluminium oxide crucible, carry out microwave heating with the crucible after three combinations at last again and handle.
Example 5
A preparation method of a high-crystallization wide-absorption carbon nitride photocatalytic material comprises the following operation steps:
(1) pressing 10g of urea in a die by using a powder tablet press to obtain a urea tablet, wherein the pressing pressure is 8 MPa;
(2) heating urea tablet with 950MHz microwave for 30min, naturally cooling to room temperature to obtain carbon nitride material named CN8-30The container when wherein urea piece microwave heating is the aluminium oxide crucible, during the microwave heating, earlier place the urea piece in first aluminium oxide crucible, then back-off a volume is the second aluminium oxide crucible 2 times of first aluminium oxide crucible on first aluminium oxide crucible, then place the crucible after the combination in the volumetric is the third aluminium oxide crucible 5 times of second aluminium oxide crucible volume, last fill up copper oxide in the third aluminium oxide crucible, cover the second aluminium oxide crucible, carry out microwave heating with the crucible after three combinations at last again and handle.
Example 6
A preparation method of a high-crystallization wide-absorption carbon nitride photocatalytic material comprises the following operation steps:
(1) pressing 10g of urea in a die by using a powder tablet press to obtain a urea tablet, wherein the pressing pressure is 8 MPa;
(2) heating urea tablet with 1000MHz microwave for 35min, naturally cooling to room temperature to obtain carbon nitride material named CN8-35The container when wherein urea piece microwave heating is the aluminium oxide crucible, during the microwave heating, earlier place the urea piece in first aluminium oxide crucible, then back-off a volume is the second aluminium oxide crucible 2 times of first aluminium oxide crucible on first aluminium oxide crucible, then place the crucible after the combination in the volumetric is the third aluminium oxide crucible 5 times of second aluminium oxide crucible volume, last fill up copper oxide in the third aluminium oxide crucible, cover the second aluminium oxide crucible, carry out microwave heating with the crucible after three combinations at last again and handle.
Example 7
A preparation method of a high-crystallization wide-absorption carbon nitride photocatalytic material comprises the following operation steps:
(1) pressing 10g of urea in a die by using a powder tablet press to obtain a urea tablet, wherein the pressing pressure is 24 MPa;
(2) heating urea tablet with 1100MHz microwave for 25min, naturally cooling to room temperature to obtain carbon nitride material named CN24-25The container when wherein urea piece microwave heating is the aluminium oxide crucible, during the microwave heating, earlier place the urea piece in first aluminium oxide crucible, then back-off a volume is the second aluminium oxide crucible 2 times of first aluminium oxide crucible on first aluminium oxide crucible, then place the crucible after the combination in the volumetric is the third aluminium oxide crucible 5 times of second aluminium oxide crucible volume, last fill up copper oxide in the third aluminium oxide crucible, cover the second aluminium oxide crucible, carry out microwave heating with the crucible after three combinations at last again and handle.
Example 8
A preparation method of a high-crystallization wide-absorption carbon nitride photocatalytic material comprises the following operation steps:
(1) pressing 10g of urea in a die by using a powder tablet press to obtain a urea tablet, wherein the pressing pressure is 24 MPa;
(2) after the urea sheet is subjected to microwave heating treatment for 30min at the frequency of 1100MHz, the urea sheet is naturally cooled to room temperature to obtain a carbon nitride material, wherein a container during microwave heating of the urea sheet is an alumina crucible, during microwave heating, the urea sheet is firstly placed in a first alumina crucible, then a second alumina crucible with the volume 2 times that of the first alumina crucible is reversely buckled on the first alumina crucible, then the combined crucible is placed in a third alumina crucible with the volume 5 times that of the second alumina crucible, finally, copper oxide is filled in the third alumina crucible, the second alumina crucible is covered, and finally, the three combined crucibles are subjected to microwave heating treatment.
Example 9
A preparation method of a high-crystallization wide-absorption carbon nitride photocatalytic material comprises the following operation steps:
(1) pressing 10g of urea in a die by using a powder tablet press to obtain a urea tablet, wherein the pressing pressure is 24 MPa;
(2) heating urea tablet with 1100MHz microwave for 35min, naturally cooling to room temperature to obtain carbon nitride material named CN24-35The container when wherein urea piece microwave heating is the aluminium oxide crucible, during the microwave heating, earlier place the urea piece in first aluminium oxide crucible, then back-off a volume is the second aluminium oxide crucible 2 times of first aluminium oxide crucible on first aluminium oxide crucible, then place the crucible after the combination in the volumetric is the third aluminium oxide crucible 5 times of second aluminium oxide crucible volume, last fill up copper oxide in the third aluminium oxide crucible, cover the second aluminium oxide crucible, carry out microwave heating with the crucible after three combinations at last again and handle.
Comparative example 1
The detailed process for preparing carbon nitride conventionally comprises the following steps: weighing 10g of urea, putting the urea into a 25mL alumina crucible, putting the alumina crucible into a muffle furnace, heating the alumina crucible at 550 ℃ for 4 hours, and naturally cooling the alumina crucible to room temperature to obtain the traditional carbon nitride material (named CN).
Example 10
A method for using a high-crystallinity wide-absorption carbon nitride photocatalytic material comprises the following operation steps:
(1) placing 10mg of carbon nitride photocatalytic material in a reactor for photocatalytic water decomposition;
(2) adding 20ml of triethanolamine aqueous solution with the mass fraction of 10% into a reactor for photocatalytic water decomposition as a sacrificial agent;
(3) adding chloroplatinic acid as a cocatalyst thereto and sealing;
(4) introducing argon into the photocatalytic water decomposition reactor, and removing air in the photocatalytic water decomposition reactor, wherein the time for introducing the argon is 15-25 min;
(5) and turning on a magnetic stirrer, turning on a light source, and carrying out a photolysis hydrogen production reaction for 4 hours, wherein the light source is a 300W xenon lamp provided with an optical filter with the wavelength of more than or equal to 420 nm.
TABLE 1 comparison of hydrogen production for high-crystalline, wide-absorption carbon nitride photocatalytic materials prepared in each example and comparative example
As can be seen from table 1, the high-crystalline and wide-absorption carbon nitride photocatalytic material obtained in example 5 is most excellent in hydrogen production effect.
The embodiments described above are some, but not all embodiments of the invention. The detailed description of the embodiments of the present invention is not intended to limit the scope of the invention as claimed, but is merely representative of selected embodiments of the invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Claims (9)
1. A preparation method of a high-crystallization wide-absorption carbon nitride photocatalytic material is characterized by comprising the following operation steps:
(1) pressing and molding urea in a die by adopting a powder tablet machine to obtain a urea tablet;
(2) and (3) heating the urea sheet by adopting 900-1100MHz frequency microwave, and naturally cooling to room temperature to obtain the carbon nitride material.
2. The method for preparing a high-crystallinity and wide-absorption carbon nitride photocatalytic material as claimed in claim 1, wherein in the step (1), the pressing pressure is 2-24 MPa.
3. The method according to claim 1, wherein in the step (2), the container for microwave heating of the urea sheet is an alumina crucible, the urea sheet is first placed in the first alumina crucible during microwave heating, then a second alumina crucible with a volume 2 times that of the first alumina crucible is reversed on the first alumina crucible, then the combined crucible is placed in a third alumina crucible with a volume 5 times that of the second alumina crucible, finally the third alumina crucible is filled with copper oxide, the second alumina crucible is covered, and finally the three combined crucibles are subjected to microwave heating treatment.
4. The method for preparing a high-crystallinity and wide-absorption carbon nitride photocatalytic material according to claim 1, wherein in the step (2), the microwave heating treatment time is 25-35 min.
5. The method for using the high-crystallinity and wide-absorption carbon nitride photocatalytic material as claimed in claim 1, is characterized by comprising the following operation steps:
(1) placing a carbon nitride photocatalytic material in a photocatalytic water decomposition reactor;
(2) adding triethanolamine aqueous solution as a sacrificial agent into a reactor for photocatalytic water decomposition;
(3) adding chloroplatinic acid as a cocatalyst thereto and sealing;
(4) introducing argon into the photocatalytic water decomposition reactor, and removing air in the photocatalytic water decomposition reactor;
(5) and (4) turning on the magnetic stirrer, turning on a light source, and carrying out the photolysis water hydrogen production reaction.
6. The method for using a high-crystallinity wide-absorption carbon nitride photocatalytic material as claimed in claim 5, wherein in the step (2), the mass fraction of triethanolamine in the triethanolamine aqueous solution is 8-12%.
7. The method for using the high-crystallinity wide-absorption carbon nitride photocatalytic material as claimed in claim 5, wherein in the step (4), the time for introducing argon is 15-25 min.
8. The method of claim 5, wherein in step (5), the light source is a 300W xenon lamp with a filter with a wavelength of 420nm or more.
9. The method for using a high-crystallinity and wide-absorption carbon nitride photocatalytic material as claimed in claim 5, wherein in the step (5), the time for the hydrogen production reaction by photolysis of water is 4-6 hours.
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
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Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104415786A (en) * | 2013-09-04 | 2015-03-18 | 安徽大学 | Method for quickly preparing quasi-graphite-structure carbon nitride material by adopting microwave heating |
| CN106542509A (en) * | 2016-10-19 | 2017-03-29 | 张家港市东大工业技术研究院 | A kind of efficient method for preparing class Graphene carbonitride |
| CN109529908A (en) * | 2019-01-13 | 2019-03-29 | 大连理工大学 | A kind of porous g-C3N4The preparation method and applications of material |
| WO2019229255A1 (en) * | 2018-05-31 | 2019-12-05 | Cambridge Enterprise Limited | Photocatalyst and photocatalytic methods for producing hydrogen |
-
2020
- 2020-12-03 CN CN202011396361.4A patent/CN112371160A/en active Pending
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104415786A (en) * | 2013-09-04 | 2015-03-18 | 安徽大学 | Method for quickly preparing quasi-graphite-structure carbon nitride material by adopting microwave heating |
| CN106542509A (en) * | 2016-10-19 | 2017-03-29 | 张家港市东大工业技术研究院 | A kind of efficient method for preparing class Graphene carbonitride |
| WO2019229255A1 (en) * | 2018-05-31 | 2019-12-05 | Cambridge Enterprise Limited | Photocatalyst and photocatalytic methods for producing hydrogen |
| CN109529908A (en) * | 2019-01-13 | 2019-03-29 | 大连理工大学 | A kind of porous g-C3N4The preparation method and applications of material |
Non-Patent Citations (1)
| Title |
|---|
| 叶萍: ""微波加热快速制备光催化材料及其可见光光催化制氢性能"", 《万方数据知识服务平台》 * |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115159477A (en) * | 2022-05-18 | 2022-10-11 | 安徽大学 | Carbon nitride material with n-pi + transition and preparation method thereof |
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