CN108543546A - The preparation method of graphite phase carbon nitride photochemical catalyst with visible light catalysis activity - Google Patents
The preparation method of graphite phase carbon nitride photochemical catalyst with visible light catalysis activity Download PDFInfo
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 87
- JMANVNJQNLATNU-UHFFFAOYSA-N oxalonitrile Chemical compound N#CC#N JMANVNJQNLATNU-UHFFFAOYSA-N 0.000 title claims abstract description 80
- 229910002804 graphite Inorganic materials 0.000 title claims abstract description 78
- 239000010439 graphite Substances 0.000 title claims abstract description 78
- 239000003054 catalyst Substances 0.000 title claims abstract description 41
- 238000006555 catalytic reaction Methods 0.000 title claims abstract description 15
- 238000002360 preparation method Methods 0.000 title claims abstract description 11
- 230000000694 effects Effects 0.000 title claims abstract description 10
- KCXVZYZYPLLWCC-UHFFFAOYSA-N EDTA Chemical compound OC(=O)CN(CC(O)=O)CCN(CC(O)=O)CC(O)=O KCXVZYZYPLLWCC-UHFFFAOYSA-N 0.000 claims abstract description 47
- 229960001484 edetic acid Drugs 0.000 claims abstract description 43
- 239000011812 mixed powder Substances 0.000 claims abstract description 21
- 238000000034 method Methods 0.000 claims abstract description 12
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- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 13
- 239000004202 carbamide Substances 0.000 claims description 13
- 229920000877 Melamine resin Polymers 0.000 claims description 10
- 238000010438 heat treatment Methods 0.000 claims description 10
- 229910052799 carbon Inorganic materials 0.000 claims description 9
- JDSHMPZPIAZGSV-UHFFFAOYSA-N melamine Chemical compound NC1=NC(N)=NC(N)=N1 JDSHMPZPIAZGSV-UHFFFAOYSA-N 0.000 claims description 9
- 238000002791 soaking Methods 0.000 claims description 2
- 230000015556 catabolic process Effects 0.000 abstract description 19
- 238000006731 degradation reaction Methods 0.000 abstract description 19
- STZCRXQWRGQSJD-GEEYTBSJSA-M methyl orange Chemical compound [Na+].C1=CC(N(C)C)=CC=C1\N=N\C1=CC=C(S([O-])(=O)=O)C=C1 STZCRXQWRGQSJD-GEEYTBSJSA-M 0.000 abstract description 12
- 229940012189 methyl orange Drugs 0.000 abstract description 12
- 238000004519 manufacturing process Methods 0.000 abstract description 3
- 238000004064 recycling Methods 0.000 abstract description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 8
- 239000000463 material Substances 0.000 description 8
- 238000005033 Fourier transform infrared spectroscopy Methods 0.000 description 6
- 239000013078 crystal Substances 0.000 description 6
- 238000010521 absorption reaction Methods 0.000 description 5
- 230000003197 catalytic effect Effects 0.000 description 5
- 230000001699 photocatalysis Effects 0.000 description 5
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 4
- 229910052757 nitrogen Inorganic materials 0.000 description 4
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 4
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 3
- 238000002835 absorbance Methods 0.000 description 3
- 230000032900 absorption of visible light Effects 0.000 description 3
- BNWPUUZJGBXAFM-UHFFFAOYSA-N azane oxalonitrile Chemical compound N.N#CC#N BNWPUUZJGBXAFM-UHFFFAOYSA-N 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 3
- 239000003795 chemical substances by application Substances 0.000 description 3
- 238000007334 copolymerization reaction Methods 0.000 description 3
- 230000003287 optical effect Effects 0.000 description 3
- PIICEJLVQHRZGT-UHFFFAOYSA-N Ethylenediamine Chemical compound NCCN PIICEJLVQHRZGT-UHFFFAOYSA-N 0.000 description 2
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- 238000005119 centrifugation Methods 0.000 description 2
- 230000007547 defect Effects 0.000 description 2
- 238000004770 highest occupied molecular orbital Methods 0.000 description 2
- 238000004768 lowest unoccupied molecular orbital Methods 0.000 description 2
- 229910052755 nonmetal Inorganic materials 0.000 description 2
- 229910052763 palladium Inorganic materials 0.000 description 2
- 229910052697 platinum Inorganic materials 0.000 description 2
- 238000000926 separation method Methods 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- XVGHZFWFGXDIOU-UHFFFAOYSA-N 2-aminothiophene-3-carbonitrile Chemical compound NC=1SC=CC=1C#N XVGHZFWFGXDIOU-UHFFFAOYSA-N 0.000 description 1
- 239000005864 Sulphur Substances 0.000 description 1
- FRTNIYVUDIHXPG-UHFFFAOYSA-N acetic acid;ethane-1,2-diamine Chemical class CC(O)=O.CC(O)=O.CC(O)=O.CC(O)=O.NCCN FRTNIYVUDIHXPG-UHFFFAOYSA-N 0.000 description 1
- 150000001412 amines Chemical class 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 238000003776 cleavage reaction Methods 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 239000000356 contaminant Substances 0.000 description 1
- 230000000593 degrading effect Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 239000002019 doping agent Substances 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 125000001153 fluoro group Chemical group F* 0.000 description 1
- 125000000623 heterocyclic group Chemical group 0.000 description 1
- 230000001788 irregular Effects 0.000 description 1
- 231100001231 less toxic Toxicity 0.000 description 1
- -1 melamine Amine Chemical class 0.000 description 1
- 238000013508 migration Methods 0.000 description 1
- 230000005012 migration Effects 0.000 description 1
- 239000000178 monomer Substances 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- 239000005416 organic matter Substances 0.000 description 1
- 238000007146 photocatalysis Methods 0.000 description 1
- 239000011941 photocatalyst Substances 0.000 description 1
- 125000004193 piperazinyl group Chemical group 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 238000013094 purity test Methods 0.000 description 1
- 239000010453 quartz Substances 0.000 description 1
- 239000000376 reactant Substances 0.000 description 1
- 230000029058 respiratory gaseous exchange Effects 0.000 description 1
- 230000007017 scission Effects 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 150000003384 small molecules Chemical class 0.000 description 1
- STZCRXQWRGQSJD-UHFFFAOYSA-M sodium;4-[[4-(dimethylamino)phenyl]diazenyl]benzenesulfonate Chemical compound [Na+].C1=CC(N(C)C)=CC=C1N=NC1=CC=C(S([O-])(=O)=O)C=C1 STZCRXQWRGQSJD-UHFFFAOYSA-M 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 231100000419 toxicity Toxicity 0.000 description 1
- 230000001988 toxicity Effects 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-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—
Abstract
A kind of preparation method of the graphite phase carbon nitride photochemical catalyst with visible light catalysis activity, carries out according to the following steps：(1) ethylenediamine tetra-acetic acid powder is mixed with aggressiveness before carbonitride and is ground uniformly, mixed-powder is made；(2) mixed-powder is warming up to 450~600 DEG C, then heat preservation carries out copolyreaction, then cools to room temperature with the furnace, and graphite phase carbon nitride photochemical catalyst is made.The method of the present invention is of low cost, meets actual production demand, simple for process, has wide economy and actual application prospect；The graphite phase carbon nitride of preparation can easily carry out separating treatment, high recycling rate with efficient degradation methyl orange in light-catalyzed reaction system.
Description
Technical field
The invention belongs to non-metal optical catalyst technical field, more particularly to a kind of graphite with visible light catalysis activity
The preparation method of phase carbon nitride photochemical catalyst.
Background technology
Graphite phase carbon nitride is a kind of novel non-metal optical catalysis material, with traditional TiO2, ZnO, the early stage such as platinum palladium
Catalysis material is compared, and the carbon of carbon nitride material and the rich reserves of nitrogen, carbon nitride material preparation process letter are formed
Single, environmental-friendly, in addition graphite phase carbon nitride material has two dimensional surface lamellar structure, therefore has very high specific surface
Product；These advantages make graphite phase carbon nitride material by the extensive concern of researcher, and light degradation environmental contaminants with
And there is potential application in the fields such as photocatalytic cleavage water.
But there is also problems for graphite phase carbon nitride；First, it is limited by own electronic structure, graphite-phase nitrogen
The band gap width for changing carbon is generally higher than 2.7ev, thus the material can only absorbing wavelength be less than the sunlight of 450nm, for the sun
Light utilization ratio is relatively low so that catalytic inner carrier concentration is low；Secondly, the hole generated after photon and photoproduction are absorbed
Electronics is easy to compound, can not be transmitted to catalyst surface and participate in light-catalyzed reaction.These disadvantages make graphite phase carbon nitride in reality
Catalytic efficiency is very low in the use of border, can not be with classical semiconductor catalyst such as TiO2And noble metal catalyst such as platinum palladium chtalyst
Agent compares.
Since the catalytic property of graphite phase carbon nitride and its own pi-conjugated electronic structure have close contact,
The electronic structure of graphite phase carbon nitride can be changed by way of doping and then regulate and control its energy gap, improve material too
Sunlight utilization, and then photoproduction carrier concentration is improved, improve the catalytic efficiency of catalyst；Meanwhile Reasonable Regulation And Control dopant
Type and content can regulate and control highest occupied molecular orbital (HOMO tracks) and lowest unoccupied molecular orbital (LUMO tracks) distribution of catalyst, promote
Into the separation of photogenerated charge and hole, the photocatalytic activity of catalyst is further increased；Seminar of king Xinchen of University of Fuzhou utilizes
Graphite phase carbon nitride (the Chinese invention patent with visible light catalysis activity is made with urea copolymerization in 2- aminothiophene -3- formonitrile HCNs
CN103272639B), the copolymerization small molecule but used in this method is expensive；Tongji University's Feng's thunderstorm et al. utilizes sulphur powder
With cyanogen ammonia hybrid reaction, it is prepared for the graphite phase carbon nitride (Chinese invention patent with the sulfur doping of photocatalytic activity
CN104056648 B), but the monomer cyanogen ammonia used in it has toxicity, and there are security risks.
Invention content
For the above problem existing for existing graphite phase carbon nitride photochemical catalyst technology of preparing, the present invention, which provides one kind, to be had
The preparation method of the graphite phase carbon nitride photochemical catalyst of visible light catalysis activity makes graphite-phase nitrogen by adulterating ethylenediamine tetra-acetic acid
Changing carbon, there is adjustable band gap width, quick photo-generated carrier separating capacity organic matter is realized under visible light conditions
Fast degradation.
The method of the present invention carries out according to the following steps：
1, ethylenediamine tetra-acetic acid powder is mixed with aggressiveness before carbonitride and is ground uniformly, mixed-powder is made；Described
Aggressiveness is urea or melamine before carbonitride；
2, mixed-powder is warming up to 450~600 DEG C, then heat preservation carries out copolyreaction, then cools to room temperature with the furnace, makes
At graphite phase carbon nitride photochemical catalyst.
The reaction equation of above-mentioned step 2 copolyreaction is：
Or it is：
In the above method, the mass ratio of aggressiveness and ethylenediamine tetra-acetic acid is 10 before carbonitride:(0.01~0.2).
In the above method, heating rate is 0.5~10 DEG C/min.
In the above method, soaking time is 1~4h.
Beneficial effects of the present invention are：
1, urea and melamine are simply less toxic compared to reactants such as cyanogen ammonia, of low cost, meet actual production demand,
It is simple for process, there is wide economy and actual application prospect；
2, the graphite phase carbon nitride prepared has adjustable band gap width, improves the absorption efficiency of visible light, simultaneously
The photo-generated carrier separation of catalytic inner, transport efficiency are improved；
3, the graphite phase carbon nitride prepared can be with efficient degradation methyl orange, relative to no copolymerization ethylenediamine tetra-acetic acid molecule
Graphite phase carbon nitride, degradation rate can be enhanced about more than once；Meanwhile prepared catalyst is in light-catalyzed reaction system
Separating treatment can be easily carried out, high recycling rate has very high practical value and is widely applied foreground.
Description of the drawings
Fig. 1 is graphite phase carbon nitride photochemical catalyst and traditional undoped ethylenediamine tetra-acetic acid in the embodiment of the present invention
The TEM photo figures of graphite phase carbon nitride；In figure, A and B are the graphite phase carbon nitride undoped with ethylenediamine tetra-acetic acid, and C and D are real
Example 2 is applied, E and F are embodiment 3；
Fig. 2 is graphite phase carbon nitride photochemical catalyst and traditional undoped ethylenediamine tetra-acetic acid in the embodiment of the present invention
The XRD diagram of graphite phase carbon nitride；In figure each curve be followed successively by from top to bottom undoped with ethylenediamine tetra-acetic acid graphite phase carbon nitride,
Embodiment 1, embodiment 2, embodiment 3 and embodiment 4；
Fig. 3 is graphite phase carbon nitride photochemical catalyst and traditional undoped ethylenediamine tetra-acetic acid in the embodiment of the present invention
The Fourier transform infrared FT-IR figures of graphite phase carbon nitride；Each curve is followed successively by from top to bottom undoped with ethylenediamine tetrem in figure
Graphite phase carbon nitride, embodiment 2 and the embodiment 4 of acid；
Fig. 4 is graphite phase carbon nitride photochemical catalyst and traditional undoped ethylenediamine tetra-acetic acid in the embodiment of the present invention
The wavelength of graphite phase carbon nitride-absorbance curve figure；Each curve is followed successively by embodiment 4, embodiment 3, implements from top to bottom in figure
Example 2, embodiment 1 and the graphite phase carbon nitride undoped with ethylenediamine tetra-acetic acid；
Fig. 5 is graphite phase carbon nitride photochemical catalyst and traditional undoped ethylenediamine tetra-acetic acid in the embodiment of the present invention
The appearance photo figure of graphite phase carbon nitride；In figure, upper row is from left to right followed successively by the graphite-phase nitrogen undoped with ethylenediamine tetra-acetic acid
Change carbon, embodiment 1 and embodiment 2, lower row is from left to right embodiment 3 and embodiment 4；
Fig. 6 is graphite phase carbon nitride photochemical catalyst and traditional undoped ethylenediamine tetra-acetic acid in the embodiment of the present invention
(the ah ν) of graphite phase carbon nitride2- h ν curve graphs；In figure, ━ is the graphite phase carbon nitride undoped with ethylenediamine tetra-acetic acid, and ★ is
Embodiment 1, ◆ it is embodiment 2, ▲ it is embodiment 3, ● it is embodiment 4；
Fig. 7 is graphite phase carbon nitride photochemical catalyst and traditional undoped ethylenediamine tetra-acetic acid in the embodiment of the present invention
The wavelength of graphite phase carbon nitride-fluorescence intensity curves figure；In figure, ━ is the graphite phase carbon nitride undoped with ethylenediamine tetra-acetic acid,
★ is embodiment 1, ◆ it is embodiment 2, ▲ it is embodiment 3, ● it is embodiment 4；
Fig. 8 is graphite phase carbon nitride photochemical catalyst and traditional undoped ethylenediamine tetra-acetic acid in the embodiment of the present invention
Degradation rate curve graph of the graphite phase carbon nitride to methyl orange；Each curve is followed successively by from top to bottom in figure does not add graphite-phase nitridation
Carbon adds the graphite phase carbon nitride undoped with ethylenediamine tetra-acetic acid, adds the product of embodiment 1, adds the product of embodiment 2,
The product of embodiment 4 is added, the product of embodiment 3 is added；
Fig. 9 is that the graphite phase carbon nitride photochemical catalyst in the embodiment of the present invention 2 reuses curve to the degradation of methyl orange
Figure；In figure, be followed successively by from left to right degradation is primary, degradation is secondary, degradation three times, degradation four times and degradation five times.
Specific implementation mode
It carries out that mixed-powder being placed in the crucible with lid when copolyreaction in the embodiment of the present invention, then in horse
Copolyreaction is not carried out in stove.
The ethylenediamine tetra-acetic acid powder purity 98% used in the embodiment of the present invention, urea crystal purity 99%, melamine
Amine purity is 99%, is Sigma Aldrich products.
The transmission electron microscope model JEOL1230 used in the embodiment of the present invention.
The model Rigaku Ultima III of the X-ray diffractometer used in the embodiment of the present invention.
The Fourier transform infrared FT-IR unit types used in the embodiment of the present invention is Vertex 80Bruket.
In the embodiment of the present invention (ah ν)2- h ν curve unit types are Cary 5000, use pattern for diffusing reflection pattern.
Test wavelength-fluorescence intensity unit type is Fluoro Max 3 in the embodiment of the present invention.
The method of product purity test is in the embodiment of the present invention：By the doped graphite phase carbon nitride photocatalysis of 0.2g/ml
Agent is put into 100ml, and in the methyl orange solution of 8mg/L, sample is made；Sample is placed in processing 1h at dark, makes up to balance；
With equipped with 400nm optical filters, intensity 100mW/cm2Light source AM1.5 simulated solar light sources, pass through the quartz of a diameter of 1cm
Window irradiates sample, and absorbance of the methyl orange when wavelength is 400nm is surveyed by Cary5000 UV, visible light infrared spectrometers, from
And judge the surplus of methyl orange.
After carrying out Degrading experiment using graphite phase carbon nitride photochemical catalyst in the embodiment of the present invention, pass through consolidating for centrifugation
After phase drying removes moisture removal, reused as graphite phase carbon nitride photochemical catalyst.
The present invention carries out contrast test using graphite phase carbon nitride of the tradition undoped with ethylenediamine tetra-acetic acid, with the application reality
The graphite phase carbon nitride photochemical catalyst applied in example 1~4 is compared；TEM photos are as shown in Figure 1, as seen from the figure, undoped with second two
The graphite phase carbon nitride of amine tetraacethyl is lamellar structure, adulterates the graphite phase carbon nitride of ethylenediamine tetra-acetic acid, symbolizes doping production
Lattice defect is given birth to, the generation of irregular holes can increase surface area, and defect can adjust visible absorption range；XRD is such as
Shown in Fig. 2, as seen from the figure, product occurs two at 13.1 ° and 27.4 ° and significantly belongs to graphite phase carbon nitride (100)
(002) diffraction maximum of crystal face；Fourier transform infrared FT-IR figures are as shown in figure 3, as seen from the figure, product is in 800cm-1Belong to
The breathing vibration of piperazine ring, 1200~1600cm-1The peak at place belongs to the stretching vibration of heterocycle, in 3200cm-1The broad peak at place is main
It is the more NH and NH not being bonded existing for nitridation carbon surface2Caused stretching vibration；Wavelength-absorbance curve such as Fig. 4 institutes
Show, as seen from the figure, undoped graphite phase carbon nitride is less than 450nm to the absorption of visible light, very low to the utilization rate of visible light,
Doped graphite phase carbon nitride, in 550nm or so, largely increases graphite phase carbon nitride and urges to the absorption of visible light
Absorption of the agent to visible light；Appearance photo as shown in figure 5, with ethylenediamine tetra-acetic acid doping increase, the color of product
Gradually deepen, it is known that the absorption region of visible light is changed；(ahν)2- h ν curves are as shown in fig. 6, undoped with state
The energy gap of graphite phase carbon nitride is 2.80ev, and with the increase of ethylenediamine tetra-acetic acid doping, current-carrying electrons migration occurs
The band gap width that required energy reduces graphite phase carbon nitride narrows, and the absorption region and utilization rate to visible light increase；By
Fig. 4,6 are it is found that doped graphite phase carbon nitride increases the absorption of visible light, and energy gap narrows；Wavelength-fluorescence is strong
Line write music as shown in fig. 7, as seen from the figure, the fluorescence intensity for adulterating the graphite phase carbon nitride photochemical catalyst of ethylenediamine tetra-acetic acid is apparent
It reduces, illustrates the separative efficiency for effectively increasing charge by adulterating carbon nitride photocatalyst；It is bent to the degradation rate of methyl orange
Line as shown in figure 8, the methyl orange for not adding graphite phase carbon nitride is hardly degraded, be added traditional graphite phase carbon nitride for
Methyl orange has certain degradation capability, reacts 5 hours, has 60% or so not degrade, relative to no doping ethylenediamine
The graphite phase carbon nitride of tetrem acid molecule, degradation capability can be increased by being doped with the graphite phase carbon nitride of ethylenediamine tetra-acetic acid, instead
5 hours undegradable percentage are answered to be respectively less than the graphite phase carbon nitride undoped with state；Wherein it is doped with 0.10g ethylenediamine tetra-acetic acids
Graphite phase carbon nitride can be enhanced about more than once for the degradation rate of methyl orange, 5 hours of reaction only have 10% or so and do not have
There is degradation；Curve is reused to the degradation of methyl orange as shown in figure 9, with the increase for reusing number, centrifugation successively is received
Doped carbonitride after collection still there is higher degradation capability, photocatalytic activity not to have great changes, explanation methyl orange
The high recycling rate of product.
Embodiment 1
Ethylenediamine tetra-acetic acid powder is mixed with urea crystal and is ground uniformly, mixed-powder, wherein urea and second is made
The mass ratio of ethylenediamine tetraacetic acid (EDTA) is 10:0.01；
Mixed-powder is warming up to 600 DEG C with the heating rate of 10 DEG C/min, then heat preservation 1h progress copolyreaction, then with
Stove is cooled to room temperature, and graphite phase carbon nitride photochemical catalyst is made.
Embodiment 2
Ethylenediamine tetra-acetic acid powder is mixed with urea crystal and is ground uniformly, mixed-powder, wherein urea and second is made
The mass ratio of ethylenediamine tetraacetic acid (EDTA) is 10:0.05；
Mixed-powder is warming up to 550 DEG C with the heating rate of 5 DEG C/min, then heat preservation 2h progress copolyreaction, then with
Stove is cooled to room temperature, and graphite phase carbon nitride photochemical catalyst is made.
Embodiment 3
Ethylenediamine tetra-acetic acid powder is mixed with urea crystal and is ground uniformly, mixed-powder, wherein urea and second is made
The mass ratio of ethylenediamine tetraacetic acid (EDTA) is 10:0.1；
Mixed-powder is warming up to 500 DEG C with the heating rate of 2 DEG C/min, then heat preservation 3h progress copolyreaction, then with
Stove is cooled to room temperature, and graphite phase carbon nitride photochemical catalyst is made.
Embodiment 4
Ethylenediamine tetra-acetic acid powder is mixed with urea crystal and is ground uniformly, mixed-powder, wherein urea and second is made
The mass ratio of ethylenediamine tetraacetic acid (EDTA) is 10:0.2；
Mixed-powder is warming up to 450 DEG C with the heating rate of 0.5 DEG C/min, 4h is then kept the temperature and carries out copolyreaction, then
It cools to room temperature with the furnace, graphite phase carbon nitride photochemical catalyst is made.
Embodiment 5
Ethylenediamine tetra-acetic acid powder is mixed with melamine and is ground uniformly, mixed-powder, wherein melamine is made
Mass ratio with ethylenediamine tetra-acetic acid is 10:0.01；
Mixed-powder is warming up to 450 DEG C with the heating rate of 0.5 DEG C/min, 4h is then kept the temperature and carries out copolyreaction, then
It cools to room temperature with the furnace, graphite phase carbon nitride photochemical catalyst is made.
Embodiment 6
Ethylenediamine tetra-acetic acid powder is mixed with melamine and is ground uniformly, mixed-powder, wherein melamine is made
Mass ratio with ethylenediamine tetra-acetic acid is 10:0.1；
Mixed-powder is warming up to 500 DEG C with the heating rate of 2 DEG C/min, then heat preservation 4h progress copolyreaction, then with
Stove is cooled to room temperature, and graphite phase carbon nitride photochemical catalyst is made.
Embodiment 7
Ethylenediamine tetra-acetic acid powder is mixed with melamine and is ground uniformly, mixed-powder, wherein melamine is made
Mass ratio with ethylenediamine tetra-acetic acid is 10:0.2；
Mixed-powder is warming up to 600 DEG C with the heating rate of 10 DEG C/min, then heat preservation 4h progress copolyreaction, then with
Stove is cooled to room temperature, and graphite phase carbon nitride photochemical catalyst is made.
Claims (4)
1. a kind of preparation method of the graphite phase carbon nitride photochemical catalyst with visible light catalysis activity, it is characterised in that by following
Step carries out：
(1) ethylenediamine tetra-acetic acid powder is mixed with aggressiveness before carbonitride and is ground uniformly, mixed-powder is made；The nitridation
Aggressiveness is urea or melamine before carbon；
(2) mixed-powder is warming up to 450~600 DEG C, then heat preservation carries out copolyreaction, then cools to room temperature with the furnace, is made
Graphite phase carbon nitride photochemical catalyst.
2. a kind of preparation side of graphite phase carbon nitride photochemical catalyst with visible light catalysis activity according to claim 1
Method, it is characterised in that the mass ratio of aggressiveness and ethylenediamine tetra-acetic acid is 10 before carbonitride in step (1):(0.01~0.2).
3. a kind of preparation side of graphite phase carbon nitride photochemical catalyst with visible light catalysis activity according to claim 1
Method, it is characterised in that the heating rate in step (2) when heating is 0.5~10 DEG C/min.
4. a kind of preparation side of graphite phase carbon nitride photochemical catalyst with visible light catalysis activity according to claim 1
Method, it is characterised in that soaking time is 1~4h in step (2).
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN111437859A (en) * | 2020-03-11 | 2020-07-24 | 浙江大学 | High-efficiency non-metal carbon-based catalyst and preparation method and application thereof |
| CN113769771A (en) * | 2021-08-16 | 2021-12-10 | 中化学朗正环保科技有限公司 | Graphite phase carbon nitride photocatalyst for sewage treatment and preparation method and application thereof |
| CN116281892A (en) * | 2023-03-07 | 2023-06-23 | 济南大学 | Visible light response type red carbon nitride and application thereof as photocatalyst |
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| CN111437859A (en) * | 2020-03-11 | 2020-07-24 | 浙江大学 | High-efficiency non-metal carbon-based catalyst and preparation method and application thereof |
| CN111437859B (en) * | 2020-03-11 | 2021-08-13 | 浙江大学 | High-efficiency non-metal carbon-based catalyst and preparation method and application thereof |
| CN113769771A (en) * | 2021-08-16 | 2021-12-10 | 中化学朗正环保科技有限公司 | Graphite phase carbon nitride photocatalyst for sewage treatment and preparation method and application thereof |
| CN113769771B (en) * | 2021-08-16 | 2023-08-25 | 中化学朗正环保科技有限公司 | Graphite-phase carbon nitride photocatalyst for sewage treatment and preparation method and application thereof |
| CN116281892A (en) * | 2023-03-07 | 2023-06-23 | 济南大学 | Visible light response type red carbon nitride and application thereof as photocatalyst |
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