CN108126729B - Graphene-like carbon nitride based composite photocatalyst and preparation method thereof - Google Patents
Graphene-like carbon nitride based composite photocatalyst and preparation method thereof Download PDFInfo
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- CN108126729B CN108126729B CN201810024793.9A CN201810024793A CN108126729B CN 108126729 B CN108126729 B CN 108126729B CN 201810024793 A CN201810024793 A CN 201810024793A CN 108126729 B CN108126729 B CN 108126729B
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- JMANVNJQNLATNU-UHFFFAOYSA-N oxalonitrile Chemical compound N#CC#N JMANVNJQNLATNU-UHFFFAOYSA-N 0.000 title claims abstract description 52
- 239000011941 photocatalyst Substances 0.000 title claims abstract description 27
- 239000002131 composite material Substances 0.000 title claims abstract description 19
- 238000002360 preparation method Methods 0.000 title claims abstract description 12
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 23
- ZKKLPDLKUGTPME-UHFFFAOYSA-N diazanium;bis(sulfanylidene)molybdenum;sulfanide Chemical compound [NH4+].[NH4+].[SH-].[SH-].S=[Mo]=S ZKKLPDLKUGTPME-UHFFFAOYSA-N 0.000 claims abstract description 10
- 239000002243 precursor Substances 0.000 claims abstract description 7
- 239000008367 deionised water Substances 0.000 claims description 16
- 229910021641 deionized water Inorganic materials 0.000 claims description 16
- 238000006243 chemical reaction Methods 0.000 claims description 15
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 14
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 14
- 239000004202 carbamide Substances 0.000 claims description 14
- 238000001816 cooling Methods 0.000 claims description 14
- 229920000877 Melamine resin Polymers 0.000 claims description 10
- JDSHMPZPIAZGSV-UHFFFAOYSA-N melamine Chemical compound NC1=NC(N)=NC(N)=N1 JDSHMPZPIAZGSV-UHFFFAOYSA-N 0.000 claims description 10
- 238000001035 drying Methods 0.000 claims description 7
- 239000002244 precipitate Substances 0.000 claims description 7
- 238000003756 stirring Methods 0.000 claims description 7
- 238000005406 washing Methods 0.000 claims description 7
- 238000005303 weighing Methods 0.000 claims description 7
- 239000012691 Cu precursor Substances 0.000 claims description 6
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 claims description 6
- QPLDLSVMHZLSFG-UHFFFAOYSA-N Copper oxide Chemical compound [Cu]=O QPLDLSVMHZLSFG-UHFFFAOYSA-N 0.000 claims description 5
- 239000005751 Copper oxide Substances 0.000 claims description 5
- 229910000431 copper oxide Inorganic materials 0.000 claims description 5
- 229910000365 copper sulfate Inorganic materials 0.000 claims description 4
- ARUVKPQLZAKDPS-UHFFFAOYSA-L copper(II) sulfate Chemical compound [Cu+2].[O-][S+2]([O-])([O-])[O-] ARUVKPQLZAKDPS-UHFFFAOYSA-L 0.000 claims description 4
- 238000010438 heat treatment Methods 0.000 claims description 3
- ORTQZVOHEJQUHG-UHFFFAOYSA-L copper(II) chloride Chemical compound Cl[Cu]Cl ORTQZVOHEJQUHG-UHFFFAOYSA-L 0.000 claims description 2
- 239000003054 catalyst Substances 0.000 abstract description 35
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 abstract description 17
- 239000001257 hydrogen Substances 0.000 abstract description 17
- 229910052739 hydrogen Inorganic materials 0.000 abstract description 17
- 239000010949 copper Substances 0.000 abstract description 9
- 230000003197 catalytic effect Effects 0.000 abstract description 8
- 230000001699 photocatalysis Effects 0.000 abstract description 6
- 238000006303 photolysis reaction Methods 0.000 abstract description 6
- 230000015843 photosynthesis, light reaction Effects 0.000 abstract description 6
- 229910052723 transition metal Inorganic materials 0.000 abstract description 3
- -1 transition metal sulfide Chemical class 0.000 abstract description 3
- 125000004122 cyclic group Chemical group 0.000 abstract description 2
- 238000001027 hydrothermal synthesis Methods 0.000 abstract description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 abstract 1
- 230000015572 biosynthetic process Effects 0.000 abstract 1
- 229910052802 copper Inorganic materials 0.000 abstract 1
- 239000005416 organic matter Substances 0.000 abstract 1
- 238000003786 synthesis reaction Methods 0.000 abstract 1
- 238000004065 wastewater treatment Methods 0.000 abstract 1
- 238000004519 manufacturing process Methods 0.000 description 15
- 239000000463 material Substances 0.000 description 9
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 7
- 229910021389 graphene Inorganic materials 0.000 description 6
- 238000000034 method Methods 0.000 description 6
- 239000002245 particle Substances 0.000 description 6
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 description 5
- 239000012798 spherical particle Substances 0.000 description 5
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 description 2
- 238000005260 corrosion Methods 0.000 description 2
- 230000007797 corrosion Effects 0.000 description 2
- 239000002114 nanocomposite Substances 0.000 description 2
- 229910000510 noble metal Inorganic materials 0.000 description 2
- 238000007146 photocatalysis Methods 0.000 description 2
- 238000004064 recycling Methods 0.000 description 2
- 229910000161 silver phosphate Inorganic materials 0.000 description 2
- 230000002195 synergetic effect Effects 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 238000000975 co-precipitation Methods 0.000 description 1
- WDHWFGNRFMPTQS-UHFFFAOYSA-N cobalt tin Chemical compound [Co].[Sn] WDHWFGNRFMPTQS-UHFFFAOYSA-N 0.000 description 1
- OIGPMFVSGDDYHS-UHFFFAOYSA-N copper sulfanylidenemolybdenum Chemical compound [S].[Cu].[Mo] OIGPMFVSGDDYHS-UHFFFAOYSA-N 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 238000013032 photocatalytic reaction Methods 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 230000007704 transition 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
-
- 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
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/04—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of inorganic compounds, e.g. ammonia
- C01B3/042—Decomposition of water
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/02—Processes for making hydrogen or synthesis gas
- C01B2203/0266—Processes for making hydrogen or synthesis gas containing a decomposition step
- C01B2203/0277—Processes for making hydrogen or synthesis gas containing a decomposition step containing a catalytic decomposition step
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/10—Catalysts for performing the hydrogen forming reactions
- C01B2203/1041—Composition of the catalyst
- C01B2203/1076—Copper or zinc-based catalysts
-
- 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
- C01B2203/1082—Composition of support materials
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
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- Engineering & Computer Science (AREA)
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Abstract
The invention discloses a graphene-like carbon nitride based composite photocatalyst, which is a supported catalyst, wherein a carrier of the catalyst is graphene-like carbon nitride, and an active load is a ternary transition metal sulfide. The catalyst is prepared from graphene-like carbon nitride, ammonium tetrathiomolybdate and a copper-containing precursor through hydrothermal reaction. The catalyst has high visible light catalytic performance and excellent cyclic use performance, and has good application prospect in the fields of hydrogen preparation by photolysis water, organic matter photocatalytic synthesis, photocatalytic wastewater treatment and the like.
Description
Technical Field
The invention relates to a graphene-like carbon nitride based composite photocatalyst and a preparation method thereof, belonging to the preparation technology of inorganic nano composite materials.
Background
Use of TiO by Takajima and Honda automotive2The photoelectrode decomposes water to prepare hydrogen or oxygen, and the semiconductor-based photocatalyst draws more and more attention in solving the global energy shortage problem and the environmental problem. Currently, a large number of photocatalysts have been successfully developed. However, most of these photocatalysts require the addition of noble metals to extend their visible light catalytic properties.
Chinese patent CN201310455691.X discloses a C3N4/Ag3PO4A preparation method of visible light photocatalytic material and an application method thereof. The patent prepares C by an ultrasonic-assisted method3N4/Ag3PO4The visible light photocatalytic material has high visible light catalytic activity, but can be recycled by additionally adding hydrogen peroxide for treatment so as to maintain the catalytic activity.
Chinese patent 201710402676.7 discloses a method for preparing a high-efficiency photocatalyst based on non-noble metal transition element sulfide. The cobalt-tin bimetallic sulfide photocatalyst is prepared by a coprecipitation method and a hydrothermal method. The catalyst has the characteristics of large specific surface area, high catalytic activity and high stability. Nevertheless, it is disadvantageous that the catalyst consists of nanosized sulphide particles, the recycling properties of which are to be further enhanced.
Therefore, the development of a novel composite sulfide photocatalyst with low cost and excellent performance has obvious theoretical guidance and practical application significance.
Disclosure of Invention
The purpose of the invention is as follows:
the invention aims to provide a graphene-like carbon nitride based composite photocatalyst and a preparation method thereof. The ternary copper molybdenum sulfide in the catalyst can fully exert the synergistic effect among transition metal sulfides; meanwhile, the sulfide is loaded on a large-size carrier, so that the recovery performance of the photocatalyst can be obviously improved, and the visible light catalytic activity and the recycling performance of the catalyst can be improved to a greater extent.
The technical scheme is as follows:
the composite material takes graphene-like carbon nitride as a carrier and takes ternary transition metal sulfide as an active load to form the graphene-like carbon nitride based nanocomposite material.
The preparation method comprises the following steps:
weighing a certain amount of nitrogen-containing precursor at room temperature, placing the nitrogen-containing precursor in a muffle furnace, heating to 450-650 ℃, heating for 2-5 h, and cooling to room temperature to obtain graphene-like carbon nitride;
and (b) at room temperature, adding the graphene-like carbon nitride prepared in the step (a) into deionized water according to the mass ratio of the deionized water to the graphene-like carbon nitride of 10: 1-100: 1, ultrasonically dispersing for 1-3 h, adding ammonium tetrathiomolybdate according to the mass ratio of the ammonium tetrathiomolybdate to the graphene-like carbon nitride of 0.01: 1-0.1: 1, adding a copper precursor according to the mass ratio of the copper precursor to the graphene-like carbon nitride of 0.01: 1-0.1: 1, stirring for reaction for 0.5-1 h, transferring the mixture into a reaction kettle, reacting for 12-36 h at 150-250 ℃, cooling to room temperature, centrifugally separating, washing precipitates by using ethanol with the mass of the graphene-like carbon nitride of 50-200 times and deionized water with the mass of the graphene-like carbon nitride of 100-500 times, and drying for 10-15 h at 50-100 ℃ to obtain the graphene-like carbon nitride-like composite photocatalyst.
In the preparation method of the graphene-like carbon nitride-based composite photocatalyst, the nitrogen-containing precursor is melamine or urea;
in the preparation method of the graphene-like carbon nitride-based composite photocatalyst, the copper precursor is one of copper oxide, copper sulfate and copper chloride.
Has the advantages that: the invention aims to provide a graphene-like carbon nitride based composite photocatalyst and a preparation method thereof. The graphene carbon nitride based composite photocatalyst has high visible light catalytic activity and cyclic use performance, and has a good application prospect in the field of photocatalysis.
The invention has the characteristics that:
(1) with Cu having a higher visible response2MoS4As an active carrier, the degree of response of the graphene-like carbon nitride to visible light can be further improved, thereby promoting the utilization efficiency of the catalyst to sunlight.
(2)Cu2MoS4And a stronger synergistic effect exists between the photocatalyst and the graphene-like carbon nitride, so that the transfer efficiency of photo-generated electrons and holes in the photocatalysis process can be improved, and the catalytic activity of the catalyst can be improved.
(3)Cu2MoS4The photocatalyst has high light corrosion resistance, and can relieve possible light corrosion of graphene-like carbon nitride in a photocatalytic reaction process, so that the recyclable performance of the photocatalyst is improved.
Detailed Description
Example 1:
weighing 5g of melamine at 25 ℃, putting the melamine into a muffle furnace, roasting the melamine at 480 ℃ for 2h, and cooling the melamine to 25 ℃ to obtain graphene-like carbon nitride;
adding 1.0g of the graphene-like carbon nitride prepared in the previous step into 20mL of deionized water at 25 ℃, ultrasonically dispersing for 1h, adding 0.03g of ammonium tetrathiomolybdate and 0.02g of copper oxide, stirring for reacting for 0.5h, transferring to a reaction kettle, reacting for 36h at 150 ℃, cooling to 25 ℃, centrifugally separating, washing precipitates with 50mL of ethanol and 100mL of deionized water in sequence, and drying for 12h at 60 ℃ to obtain the graphene-like carbon nitride-based composite photocatalyst.
The carrier graphene carbon nitride in the supported catalyst is of a sheet structure, and the supported material Cu2MoS4The catalyst is spherical particles with the average particle size of 20nm, the average hydrogen production rate of the catalyst is 92mmol/h when the catalyst is applied to the hydrogen production reaction by photolysis of water under visible light, and the hydrogen production rate can still be maintained at 85mmol/h after the catalyst is continuously and circularly reacted for 5 times.
Example 2:
weighing 5g of urea at 25 ℃, putting the urea into a muffle furnace, roasting the urea for 2.5h at 500 ℃, and cooling the urea to 25 ℃ to obtain graphene-like carbon nitride;
adding 1.5g of the graphene-like carbon nitride prepared in the step into 30mL of deionized water at 25 ℃, ultrasonically dispersing for 1.5h, adding 0.045g of ammonium tetrathiomolybdate and 0.06g of copper sulfate, stirring for reaction for 1h, transferring into a reaction kettle, reacting for 30h at 180 ℃, cooling to 25 ℃, centrifugally separating, washing precipitates with 100mL of ethanol and 200mL of deionized water in sequence, and drying for 12h at 60 ℃ to obtain the graphene-like carbon nitride-based composite photocatalyst.
The carrier graphene carbon nitride in the supported catalyst is of a sheet structure, and the supported material Cu2MoS4The catalyst is spherical particles with the average particle size of 15nm, the average hydrogen production rate of the catalyst is 105mmol/h when the catalyst is applied to the hydrogen production reaction by photolysis of water under visible light, and the hydrogen production rate can still be maintained at 94mmol/h after the catalyst is continuously and circularly reacted for 5 times.
Example 3:
weighing 10g of melamine at 25 ℃, putting the melamine into a muffle furnace, roasting the melamine for 3 hours at 550 ℃, and cooling the melamine to 25 ℃ to obtain graphene-like carbon nitride;
adding 2.0g of the graphene-like carbon nitride prepared in the step into 40mL of deionized water at 25 ℃, ultrasonically dispersing for 1h, adding 0.06g of ammonium tetrathiomolybdate and 0.04g of copper oxide, stirring for reacting for 2h, transferring into a reaction kettle, reacting for 25h at 200 ℃, cooling to 25 ℃, centrifugally separating, washing precipitates with 120mL of ethanol and 240mL of deionized water in sequence, and drying for 12h at 60 ℃ to obtain the graphene-like carbon nitride composite photocatalyst.
The carrier graphene carbon nitride in the supported catalyst is of a sheet structure, and the supported material Cu2MoS4The catalyst is spherical particles with the average particle size of 12nm, the average hydrogen production rate of the catalyst is 112mmol/h when the catalyst is applied to the hydrogen production reaction by photolysis of water under visible light, and the hydrogen production rate can still be maintained at 105mmol/h after the catalyst is continuously and circularly reacted for 5 times.
Example 4:
weighing 10g of urea at 25 ℃, putting the urea into a muffle furnace, roasting the urea for 3.5 hours at 600 ℃, and cooling the urea to 25 ℃ to obtain graphene-like carbon nitride;
adding 2.5g of the graphene-like carbon nitride prepared in the step into 50mL of deionized water at 25 ℃, ultrasonically dispersing for 1.5h, adding 0.08g of ammonium tetrathiomolybdate and 0.05g of copper sulfate, stirring for reacting for 2.5h, transferring into a reaction kettle, reacting for 20h at 220 ℃, cooling to 25 ℃, centrifugally separating, washing precipitates with 150mL of ethanol and 300mL of deionized water in sequence, and drying for 12h at 60 ℃ to obtain the graphene-like carbon nitride composite photocatalyst.
The carrier graphene carbon nitride in the supported catalyst is of a sheet structure, and the supported material Cu2MoS4The catalyst is spherical particles with the average particle size of 10nm, the average hydrogen production rate of the catalyst is 118mmol/h when the catalyst is applied to the hydrogen production reaction by photolysis of water under visible light, and the hydrogen production rate can still be maintained at 109mmol/h after the catalyst is continuously and circularly reacted for 5 times.
Example 5:
weighing 10g of urea at 25 ℃, putting the urea into a muffle furnace, roasting the urea for 4 hours at 650 ℃, and cooling the urea to 25 ℃ to obtain graphene-like carbon nitride;
adding 3.0g of the graphene-like carbon nitride prepared in the step into 40mL of deionized water at 25 ℃, ultrasonically dispersing for 1h, adding 0.1g of ammonium tetrathiomolybdate and 0.08g of copper oxide, stirring for reacting for 3h, transferring into a reaction kettle, reacting for 12h at 250 ℃, cooling to 25 ℃, centrifugally separating, washing precipitates with 200mL of ethanol and 400mL of deionized water in sequence, and drying for 12h at 60 ℃ to obtain the graphene-like carbon nitride composite photocatalyst.
The carrier graphene carbon nitride in the supported catalyst is of a sheet structure, and the supported material Cu2MoS4The catalyst is spherical particles with the average particle size of 24nm, the average hydrogen production rate of the catalyst is 76mmol/h when the catalyst is applied to the hydrogen production reaction by photolysis of water under visible light, and the hydrogen production rate can still be maintained at 67mmol/h after the catalyst is continuously and circularly reacted for 5 times.
Claims (1)
1. The preparation method of the graphene-like carbon nitride based composite photocatalyst is characterized by comprising the following steps of:
step (a): weighing a certain amount of nitrogen-containing precursor at room temperature, placing the nitrogen-containing precursor in a muffle furnace, heating to 450-650 ℃, roasting for 2-5 h, and cooling to room temperature to obtain graphene-like carbon nitride;
step (b): adding the graphene-like carbon nitride prepared in the step (a) into deionized water according to the mass ratio of the deionized water to the graphene-like carbon nitride of 10: 1-100: 1 at room temperature, ultrasonically dispersing for 1-3 h, adding ammonium tetrathiomolybdate according to the mass ratio of the ammonium tetrathiomolybdate to the graphene-like carbon nitride of 0.01: 1-0.1: 1, adding a copper precursor according to the mass ratio of the copper precursor to the graphene-like carbon nitride of 0.01: 1-0.1: 1, stirring for reaction for 0.5-1 h, transferring into a reaction kettle, reacting for 12-36 h at 150-250 ℃, cooling to room temperature, centrifugally separating, washing precipitates by using ethanol with the mass of the graphene-like carbon nitride of 50-200 times and deionized water with the mass of the graphene-like carbon nitride of 100-500 times in sequence, and drying for 10-15 h at 50-100 ℃ to obtain the graphene-like carbon nitride composite photocatalyst;
wherein the nitrogen-containing precursor in the step (a) is melamine or urea;
the copper precursor in the step (b) is one of copper oxide, copper sulfate and copper chloride.
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CN109759108B (en) * | 2018-11-19 | 2021-07-20 | 江苏大学 | Ternary composite photocatalyst, preparation method and application |
CN109468662B (en) * | 2018-12-11 | 2021-04-20 | 温州大学 | Preparation method of copper-molybdenum composite material and application of copper-molybdenum composite material in catalyst for hydrogen evolution through water electrolysis |
CN111330611A (en) * | 2018-12-19 | 2020-06-26 | 南京理工大学 | Graphene-modified prismatic carbon nitride, and preparation method and application thereof |
CN111610238A (en) * | 2019-04-09 | 2020-09-01 | 中国医学科学院基础医学研究所 | Preparation method and application of copper oxide/carbon nitride-based enzyme-free glucose sensor |
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