CN109999882A - A kind of carbon quantum dot-graphite phase carbon nitride composite material, preparation method and application - Google Patents
A kind of carbon quantum dot-graphite phase carbon nitride composite material, preparation method and application Download PDFInfo
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- 238000000034 method Methods 0.000 claims abstract description 16
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- SEEPANYCNGTZFQ-UHFFFAOYSA-N sulfadiazine Chemical compound C1=CC(N)=CC=C1S(=O)(=O)NC1=NC=CC=N1 SEEPANYCNGTZFQ-UHFFFAOYSA-N 0.000 description 4
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- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
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- 239000002023 wood Substances 0.000 description 1
- 229910052724 xenon Inorganic materials 0.000 description 1
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 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—
-
- 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
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/08—Heat treatment
-
- 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
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/08—Heat treatment
- B01J37/10—Heat treatment in the presence of water, e.g. steam
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/34—Organic compounds containing oxygen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/38—Organic compounds containing nitrogen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/40—Organic compounds containing sulfur
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/10—Photocatalysts
Abstract
The present invention relates to a kind of carbon quantum dot-graphite phase carbon nitride composite materials, preparation method and application.Ascorbic acid is mixed in aqueous solution with ethylene glycol, carbon quantum dot is prepared using hydro-thermal method；The carbon quantum dot solution of preparation is diluted 100 times；Carbon quantum dot solution after dilution is mixed with urea；Above-mentioned mixed liquor is calcined using calcination method, prepares carbon quantum dot-graphite phase carbon nitride composite photo-catalyst；The composite photo-catalyst is placed in certain PPCPs solution, magnetic agitation is carried out under the irradiation of visible light.Carbon quantum dot of the invention-graphite phase carbon nitride composite material photo-catalysis capability is strong, can catalysis oxidation removal including with the various poisonous and hazardous organic micro-pollutants difficult to degrade including drug and personal care articles.
Description
Technical field
The present invention relates to a kind of carbon quantum dot-graphite phase carbon nitride composite materials, preparation method and application.
Background technique
With the whole world high speed development, people gradually recognize environmental pollution and energy shortage have become restrict the mankind can
The big major issue of the two of sustainable development.Therefore, searching and exploitation nonpollution environment recovery technique and the clean and environmental protection energy have become
The important emergency task of human social.In various green energy resources and renewable energy, semiconductor light
Catalysis technique is due to being developing progressively a kind of most potential novel skill using sunlight or artificial light and abundance
Art.From discovery TiO in 19702Since decomposing water as electrode, conductor photocatalysis is as a kind of environmentally protective technology, extensively
It is general applied to the removal and degradation of organic matter, Water warfare and disinfection.In the past few decades, due to titanium dioxide is cheap,
Chemical property is excellent and photochemical stable, has developed the photochemical catalyst largely based on titanium dioxide, is applied to environment
Contamination control.However, the bandwidth of titanium dioxide is 3.2eV, only to ultraviolet light response, and ultraviolet light is in entire solar spectrum
Only account for 4%, it is seen that light energy can reach 43% in solar energy.Therefore, find it is a kind of novelly, using visible light
Catalysis material be particularly important.
Carbonitride (C3N4) polymer can trace back to 1834, but it is graphitized carbonitride (g-C3N4) it is used as out-phase
Catalyst was risen in 2006.2009, Wang etc. utilized g-C for the first time3N4As environmentally friendly photochemical catalyst hydrogen manufacturing.
Then, it is widely studied in semiconductor light-catalyst field.It polymerize g-C3N4It is carbon and the nitrogen member by rich content on the earth
Element composition, its surface-active can improve by a variety of methods, and its main structure and ingredient it is substantially constant.g-
C3N4Contain sp2The carbon and nitrogen of hydridization, constitute pi-conjugated electronic structure, compared to TiO2, its forbidden band width is 2.7-
2.8eV, therefore the visible light near 450-460nm can be absorbed.In addition, g-C3N4Also there is very strong chemical stability, no
It is dissolved in acid, alkali and organic solvent, is a kind of stable compound[29].Based on These characteristics, g-C3N4It is that one kind has prospect very much
Environmentally friendly photochemical catalyst.However, g-C3N4From practical application also some obstacles, as the high recombination rate of hole-electronics pair,
Low conductivity and visible absorption spectrum are narrow.Carbon quantum dot possesses conjugated pi structure and becomes outstanding electronics carrier and connect
Device is received, and carbon quantum dot also possesses the characteristic for converting long wavelength light as short-wavelength light, these features can be used to be modified just
g-C3N4, to enhance g-C3N4Photocatalysis efficiency.
PPCPs is english abbreviation (the pharmaceuticals and personal care of drug and personal care articles
), products subsequent PPCPs is widely accepted as the proper noun of drug and personal care articles.PPCPs pollutant
With stronger persistence, bioaccumulation and eco-toxicity, the materialization of aquatile or biochemical reaction function can be made to change
Become, also will increase the drug resistance of human pathogen bacterium.PPCPs is in surface water, underground water, drinking water, sewage treatment plant, deposit
It is constantly detected in equal surrounding mediums, causes extensive concern both domestic and external.Therefore, it needs a kind of environmental-friendly and can utilize
The water treatment technology of sunlight handles PPCPs.
Carbon quantum dot and g-C3N4Contained element is all that content is very abundant on the earth, the modified g-C of carbon quantum dot3N4It can be with
Widen g-C3N4The range of visible light is absorbed, and accelerates the separation of electron-hole pair, to improve g-C3N4Catalytic activity.
Summary of the invention
In view of the deficiencies of the prior art, the present invention provides a kind of carbon quantum dot-graphite phase carbon nitride composite material, preparation side
It is multiple to promote carbon quantum dot-graphite phase carbon nitride to obtain epitaxial growth type carbon quantum dot-graphite phase carbon nitride composite material for method
The photocatalysis performance of condensation material；In addition, the application also provides the application of the carbon quantum dot-graphite phase carbon nitride composite material.
In order to solve the above-mentioned technical problem, technical scheme is as follows:
A kind of preparation method of carbon quantum dot-graphite phase carbon nitride composite material, includes the following steps:
S1, preparation carbon quantum dot solution, are diluted with water, obtain carbon quantum dot dilution；
S2, the S1 carbon quantum dot dilution obtained is uniformly mixed with urea, obtains mixed liquor；
S3, calcination processing is carried out to the mixed liquor that S2 is obtained, obtains carbon quantum dot-graphite phase carbon nitride composite material；
Wherein, calcination processing temperature is 500-600 DEG C, and the calcination processing time is 1.5-4.5h.
Further, in S1, using ascorbic acid and dihydric alcohol as raw material, carbon quantum dot solution is prepared by hydro-thermal method；It is excellent
Selection of land, the dihydric alcohol are ethylene glycol.
Further, in S1, ascorbic acid, ethylene glycol, water are uniformly mixed, under conditions of 140-180 DEG C, reaction
60-80min, cooling, preferably natural cooling obtain carbon quantum dot solution；
Wherein, ascorbic acid, ethylene glycol mass volume ratio be 1-2g:10-20mL, generally 1.2-1.8g:12-
The volume ratio of 18mL, ethylene glycol and water is 10-20:20-30, generally 12-18:22-28.
Preferably, in S1,80-120 times is diluted, it is further preferred that 90-110 times of dilution.
Further, under the conditions of 150-170 DEG C, 65-75min is reacted.
Further, in S2, the volume mass ratio of carbon quantum dot dilution and urea are as follows: 1.5-4.5mL:6-14g, generally
2-4mL:8-12g, preferably 3mL:10g.
Further, in S3, calcination processing process carries out in Muffle furnace.Before calcination processing, with the heating of 0.5 DEG C/min
Rate is heated to 500-600 DEG C.
Further, in S3, after the completion of calcination processing, natural cooling obtains carbon quantum dot-graphite phase carbon nitride composite wood
Material.
A kind of carbon quantum dot-graphite phase carbon nitride composite material, is made of preparation method as described above.
Carbon quantum dot-graphite phase carbon nitride composite material of preparation method preparation as described above or carbon amounts as described above
Sub- point-application of the graphite phase carbon nitride composite material as catalysis material.
Further, the carbon quantum dot-graphite phase carbon nitride composite material is placed in the solution containing PPCPs,
It is stirred under the irradiation of visible light, it is preferable that the whipping process is magnetic agitation.
Further, 0.5-5g carbon quantum dot-graphite phase carbon nitride composite material is added in solution described in every 1L.
Further, in whipping process, the temperature for controlling the solution is 10-45 DEG C.
Further, the PPCPs includes drug and personal care articles, further, including all kinds of antibiotic, artificial is closed
At Moschus, anodyne, depressor, contraceptive, somnifacient, slimming drugs, hair jelly, hair dye and fungicide etc..
The present invention generates hole-by utilizing excited by visible light carbon quantum dot-graphite phase carbon nitride (C-CN) composite material
Electronics pair, light induced electron generates superoxide radical in conjunction with oxygen, and then generates hydroxyl radical free radical, and superoxide radical, hydroxyl are certainly
It is common to aoxidize PPCPs class organic pollutant by base and photohole, it is shown below:
With other TiO2Class and g-C3N4Class photochemical catalyst is compared, the invention has the advantages that the carbon amounts that (1) is of the invention
In sub- point-graphite phase carbon nitride composite material, graphite phase carbon nitride growth in situ is in carbon quantum dot periphery, this growth course hair
In the same plane, the two is tightly combined for life；(2) the modified g-C of carbon quantum dot3N4G-C can be widened3N4Absorb visible light
Range, and accelerate the separation of electron-hole pair, to improve g-C3N4Catalytic activity；(3) carbon quantum dot-graphite-phase nitridation
Carbon composite belongs to the green material without heavy metal, will not bring secondary pollution.
Detailed description of the invention
Fig. 1 is the transmission electron microscope picture in carbon quantum dot solution thereon (left side) and carbon quantum dot.
Fig. 2 is carbon quantum dot-graphite phase carbon nitride compound transmission electron microscope picture.
Fig. 3 is graphite phase carbon nitride and carbon quantum dot-graphite phase carbon nitride compound Raman spectrogram.
Fig. 4 is that gained carbon quantum dot-graphite phase carbon nitride compound synthetic route chart is calculated using DFT.
Fig. 5 be carbon quantum dot-graphite phase carbon nitride photochemical catalyst, graphite phase carbon nitride photochemical catalyst visible light irradiation
The effect picture of lower degradation sulphadiazine.
Fig. 6 is the carbon quantum dot/g-C synthesized using conventional hydrothermal method3N4Composite material is compound with use this method preparation
The light degradation property contrast effect figure of material.
Specific embodiment
The present invention will be further described with reference to the accompanying drawing, but embodiments of the present invention are not limited to this.
Embodiment 1
The preparation of carbon quantum dot-graphite phase carbon nitride composite material:
1) 1.6g ascorbic acid is weighed, is dissolved in 25mL ultrapure water, 15ml ethylene glycol is added.By the mixed solution magnetic
Power, which stirs 30 minutes, dissolves it sufficiently, is then added in the stainless steel autoclave that 100mL liner is polytetrafluoroethylene (PTFE),
Reaction kettle is put into baking oven, be warming up to 160 DEG C and keeps 70min, then cooled to room temperature, by the carbon amounts of above-mentioned preparation
Son point solution dilutes 100 times, obtains carbon quantum dot dilution, spare.
2) 10g urea is weighed in the porcelain crucible of 50ml, and 3ml carbon quantum dot dilution is added, adds 2ml ultrapure water, stirs
Mixing mixes it uniformly, is placed in Muffle furnace, is heated to 550 DEG C, then constant temperature 3h with the heating rate of 0.5 DEG C/min, finally certainly
It so is cooled to room temperature, obtains carbon quantum dot-graphite phase carbon nitride composite material.
Embodiment 2
The method of PPCPs in the carbon quantum dot-graphite phase carbon nitride composite degradation water obtained using embodiment 1, tool
Steps are as follows for body: prepare the aqueous solution to be processed containing sulphadiazine as solution to be processed (pH=5.7), volume 60mL,
Initial sulphadiazine concentration be 10 μM (wherein, M, that is, mol/L, μM i.e. 10-6Mol/L, mM i.e. 10-3Mol/L, similarly hereinafter), it adds
Composite photo-catalyst 30mg (mass concentration 0.5g/l).With xenon lamp plus optical filter (λ > 420nm, 100w/m2) do visible light light
Mixed liquor is irradiated in source, and under room temperature after magnetic agitation 80min, up to 92.7%, effect is substantially better than sulphadiazine removal rate
Pure light group and graphite-phase nitridation charcoal processing group (referring to Fig. 5).In addition, Fig. 6 compared the carbon amounts using the synthesis of conventional hydrothermal method
Sub- point/g-C3N4The light degradation property of composite material, the composite material prepared using this method, it is clear that prepared using this method
Composite photo-catalyst have stronger contaminant degradation ability.
The carbon quantum dot solution for preparing yellow by hydro-thermal method by ascorbic acid and ethylene glycol first, such as Fig. 1 (left side) institute
Show.Fig. 1 (right side) is the transmission electron microscope picture of carbon quantum dot, it can be seen that its size is about 3nm.Fig. 2 is carbon quantum dot-stone
The transmission electron microscope picture of black phase carbon nitride compound, it can be seen that its shape is as regular hexagon and size is about 20nm.This be by
In graphite phase carbon nitride carbon quantum dot periphery growth in situ reason.Fig. 3 is graphite phase carbon nitride and carbon quantum dot-graphite
The Raman spectrogram of phase carbon nitride compound, it can be seen that compared to graphite phase carbon nitride, carbon quantum dot-graphite phase carbon nitride is multiple
The Raman spectrogram for closing object has more two characteristic peaks (peak D and the peak G) of carbon quantum dot, shows that carbon quantum dot-graphite phase carbon nitride is multiple
Closing object to be includes carbon quantum dot structure and graphite phase carbon nitride structure.Fig. 4 is carbon quantum dot-graphite phase carbon nitride compound
Synthetic route chart, by using VASP software carry out DFT calculating, show that carbon quantum dot-graphite phase carbon nitride of the application is multiple
Closing object has smaller band gap and bigger local carrier density.Carbon quantum dot/the g-C prepared using conventional hydrothermal method3N4It is compound
Material, two kinds of materials are usually combined by Van der Waals force, and use carbon quantum dot-graphite phase carbon nitride of this method synthesis multiple
Close object, between be that interatomic bond is closed, therefore has better photo-generated carrier transmission capacity, stronger photocatalysis work
Property.
The content that above-described embodiment illustrates should be understood as that these embodiments are only used for being illustrated more clearly that the present invention, without
For limiting the scope of the invention, after the present invention has been read, those skilled in the art are to various equivalent forms of the invention
Modification each fall within the application range as defined in the appended claims.
Claims (10)
1. a kind of carbon quantum dot-graphite phase carbon nitride composite material preparation method, which comprises the steps of:
S1, preparation carbon quantum dot solution, are diluted with water, obtain carbon quantum dot dilution；
S2, the S1 carbon quantum dot dilution obtained is uniformly mixed with urea, obtains mixed liquor；
S3, calcination processing is carried out to the mixed liquor that S2 is obtained, obtains carbon quantum dot-graphite phase carbon nitride composite material；
Wherein, calcination processing temperature is 500-600 DEG C, and the calcination processing time is 1.5-4.5h.
2. preparation method according to claim 1, which is characterized in that in S1, using ascorbic acid and dihydric alcohol as raw material, lead to
Cross hydro-thermal method preparation carbon quantum dot solution；Preferably, the dihydric alcohol is ethylene glycol.
3. preparation method according to claim 1, which is characterized in that in S1, ascorbic acid, ethylene glycol, water are mixed equal
It is even, under conditions of 140-180 DEG C, 60-80min is reacted, it is cooling, obtain carbon quantum dot solution；
Wherein, ascorbic acid, ethylene glycol mass volume ratio be 1-2g:10-20mL, the volume ratio of ethylene glycol and water is 10-20:
20-30。
4. preparation method according to claim 1, which is characterized in that in S2, the volume matter of carbon quantum dot dilution and urea
Measure ratio are as follows: 1.5-4.5mL:6-14g.
5. preparation method according to claim 1, which is characterized in that in S3, calcination processing process carries out in Muffle furnace,
Preferably, before calcination processing, 500-600 DEG C is heated to the heating rate of 0.5 DEG C/min.
6. a kind of carbon quantum dot-graphite phase carbon nitride composite material, which is characterized in that as described in claim any one of 1-5
Preparation method be made.
7. carbon quantum dot-graphite phase carbon nitride composite material of preparation method as described in any one in claim 1-5 preparation or
Carbon quantum dot-application of the graphite phase carbon nitride composite material as catalysis material as claimed in claim 6.
8. application according to claim 7, which is characterized in that by the carbon quantum dot-graphite phase carbon nitride composite material
It is placed in the solution containing PPCPs, is stirred under the irradiation of visible light.
9. application according to claim 8, which is characterized in that add 0.5-5g carbon quantum dot-stone in solution described in every 1L
Black phase carbon nitride composite material.
10. application according to claim 8, which is characterized in that in whipping process, the temperature for controlling the solution is 10-
45 ℃。
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