CN110270364A - A kind of support type graphite phase carbon nitride composite material, preparation method and applications - Google Patents
A kind of support type graphite phase carbon nitride composite material, preparation method and applications Download PDFInfo
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- CN110270364A CN110270364A CN201910643102.8A CN201910643102A CN110270364A CN 110270364 A CN110270364 A CN 110270364A CN 201910643102 A CN201910643102 A CN 201910643102A CN 110270364 A CN110270364 A CN 110270364A
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- carbon nitride
- phase carbon
- graphite phase
- composite material
- support type
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- JMANVNJQNLATNU-UHFFFAOYSA-N oxalonitrile Chemical compound N#CC#N JMANVNJQNLATNU-UHFFFAOYSA-N 0.000 title claims abstract description 42
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 41
- 239000010439 graphite Substances 0.000 title claims abstract description 40
- 229910002804 graphite Inorganic materials 0.000 title claims abstract description 40
- 239000002131 composite material Substances 0.000 title claims abstract description 28
- 238000002360 preparation method Methods 0.000 title claims description 15
- 239000000843 powder Substances 0.000 claims abstract description 21
- 229960000907 methylthioninium chloride Drugs 0.000 claims abstract description 18
- 230000015556 catabolic process Effects 0.000 claims abstract description 14
- 238000006731 degradation reaction Methods 0.000 claims abstract description 14
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 14
- 239000008367 deionised water Substances 0.000 claims abstract description 11
- 229910021641 deionized water Inorganic materials 0.000 claims abstract description 10
- 229910052596 spinel Inorganic materials 0.000 claims abstract description 10
- 239000011029 spinel Substances 0.000 claims abstract description 10
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims abstract description 8
- 229960000935 dehydrated alcohol Drugs 0.000 claims abstract description 8
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims abstract description 5
- 239000004202 carbamide Substances 0.000 claims abstract description 5
- RBTBFTRPCNLSDE-UHFFFAOYSA-N 3,7-bis(dimethylamino)phenothiazin-5-ium Chemical compound C1=CC(N(C)C)=CC2=[S+]C3=CC(N(C)C)=CC=C3N=C21 RBTBFTRPCNLSDE-UHFFFAOYSA-N 0.000 claims abstract 6
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 12
- CHQMHPLRPQMAMX-UHFFFAOYSA-L sodium persulfate Chemical compound [Na+].[Na+].[O-]S(=O)(=O)OOS([O-])(=O)=O CHQMHPLRPQMAMX-UHFFFAOYSA-L 0.000 claims description 12
- 238000006243 chemical reaction Methods 0.000 claims description 6
- 238000010438 heat treatment Methods 0.000 claims description 5
- CDBYLPFSWZWCQE-UHFFFAOYSA-L Sodium Carbonate Chemical group [Na+].[Na+].[O-]C([O-])=O CDBYLPFSWZWCQE-UHFFFAOYSA-L 0.000 claims description 4
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 4
- 238000001354 calcination Methods 0.000 claims description 4
- 230000007935 neutral effect Effects 0.000 claims description 4
- 239000013049 sediment Substances 0.000 claims description 4
- 229910052742 iron Inorganic materials 0.000 claims description 3
- 229910052759 nickel Inorganic materials 0.000 claims description 3
- 230000035484 reaction time Effects 0.000 claims description 3
- 150000001875 compounds Chemical class 0.000 claims description 2
- 239000000463 material Substances 0.000 claims description 2
- 239000004575 stone Substances 0.000 claims description 2
- 238000005406 washing Methods 0.000 claims description 2
- 239000000243 solution Substances 0.000 claims 5
- 229910003271 Ni-Fe Inorganic materials 0.000 claims 2
- 229910002554 Fe(NO3)3·9H2O Inorganic materials 0.000 claims 1
- 229910052799 carbon Inorganic materials 0.000 claims 1
- 238000001816 cooling Methods 0.000 claims 1
- 239000011259 mixed solution Substances 0.000 claims 1
- 238000002156 mixing Methods 0.000 claims 1
- 239000011148 porous material Substances 0.000 claims 1
- 238000010792 warming Methods 0.000 claims 1
- 238000000034 method Methods 0.000 abstract description 8
- JRKICGRDRMAZLK-UHFFFAOYSA-L peroxydisulfate Chemical compound [O-]S(=O)(=O)OOS([O-])(=O)=O JRKICGRDRMAZLK-UHFFFAOYSA-L 0.000 abstract description 6
- 230000003197 catalytic effect Effects 0.000 abstract description 4
- 230000003647 oxidation Effects 0.000 abstract description 4
- 238000007254 oxidation reaction Methods 0.000 abstract description 4
- 230000004913 activation Effects 0.000 abstract description 2
- 238000005516 engineering process Methods 0.000 abstract description 2
- 230000003213 activating effect Effects 0.000 abstract 1
- 230000015572 biosynthetic process Effects 0.000 abstract 1
- 239000003054 catalyst Substances 0.000 abstract 1
- 239000011159 matrix material Substances 0.000 abstract 1
- 238000003786 synthesis reaction Methods 0.000 abstract 1
- 239000012071 phase Substances 0.000 description 21
- CXKWCBBOMKCUKX-UHFFFAOYSA-M methylene blue Chemical compound [Cl-].C1=CC(N(C)C)=CC2=[S+]C3=CC(N(C)C)=CC=C3N=C21 CXKWCBBOMKCUKX-UHFFFAOYSA-M 0.000 description 12
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 10
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 10
- 239000011157 advanced composite material Substances 0.000 description 10
- 239000000975 dye Substances 0.000 description 10
- 239000002351 wastewater Substances 0.000 description 5
- 239000002184 metal Substances 0.000 description 3
- 229910052751 metal Inorganic materials 0.000 description 3
- 239000011943 nanocatalyst Substances 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- 238000004833 X-ray photoelectron spectroscopy Methods 0.000 description 2
- 230000005540 biological transmission Effects 0.000 description 2
- 238000006555 catalytic reaction Methods 0.000 description 2
- 239000002082 metal nanoparticle Substances 0.000 description 2
- 230000008569 process Effects 0.000 description 2
- 239000000454 talc Substances 0.000 description 2
- 229910052623 talc Inorganic materials 0.000 description 2
- 235000012222 talc Nutrition 0.000 description 2
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 125000003118 aryl group Chemical group 0.000 description 1
- 239000000981 basic dye Substances 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 239000002537 cosmetic Substances 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000002242 deionisation method Methods 0.000 description 1
- GDVKFRBCXAPAQJ-UHFFFAOYSA-A dialuminum;hexamagnesium;carbonate;hexadecahydroxide Chemical compound [OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Al+3].[Al+3].[O-]C([O-])=O GDVKFRBCXAPAQJ-UHFFFAOYSA-A 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 239000003814 drug Substances 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 229910001701 hydrotalcite Inorganic materials 0.000 description 1
- 229960001545 hydrotalcite Drugs 0.000 description 1
- 238000005342 ion exchange Methods 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 238000011068 loading method Methods 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000005297 material degradation process Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 239000002086 nanomaterial Substances 0.000 description 1
- 239000000049 pigment Substances 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 238000005245 sintering Methods 0.000 description 1
- 239000007790 solid phase Substances 0.000 description 1
- 239000004753 textile Substances 0.000 description 1
- 231100000331 toxic Toxicity 0.000 description 1
- 230000002588 toxic effect Effects 0.000 description 1
- 238000004065 wastewater treatment Methods 0.000 description 1
Classifications
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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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/007—Mixed salts
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/24—Nitrogen compounds
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/20—Catalysts, in general, characterised by their form or physical properties characterised by their non-solid state
- B01J35/23—Catalysts, in general, characterised by their form or physical properties characterised by their non-solid state in a colloidal state
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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
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/30—Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
- B01J35/39—Photocatalytic properties
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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
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/30—Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
- B01J35/396—Distribution of the active metal ingredient
- B01J35/399—Distribution of the active metal ingredient homogeneously throughout the support particle
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/60—Catalysts, in general, characterised by their form or physical properties characterised by their surface properties or porosity
- B01J35/61—Surface area
- B01J35/613—10-100 m2/g
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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
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/60—Catalysts, in general, characterised by their form or physical properties characterised by their surface properties or porosity
- B01J35/64—Pore diameter
- B01J35/651—50-500 nm
-
- 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
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
- C02F1/725—Treatment of water, waste water, or sewage by oxidation by catalytic oxidation
-
- 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
- C02F2101/308—Dyes; Colorants; Fluorescent agents
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- 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
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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
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W10/00—Technologies for wastewater treatment
- Y02W10/30—Wastewater or sewage treatment systems using renewable energies
- Y02W10/37—Wastewater or sewage treatment systems using renewable energies using solar energy
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- Carbon And Carbon Compounds (AREA)
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Abstract
The invention belongs to a kind of support type graphite phase carbon nitride composite material, composite material is that stratiform nickel-ferric spinel (NiFe-LDH) loads graphite phase carbon nitride and its application for activating persulfate oxidation degradation of methylene blue.The present invention uses two-step method synthetic technology, first by a certain amount of urea grind into powder, synthesis porous graphite phase carbon nitride is handled by pyrocondensation, then it is washed repeatedly using dehydrated alcohol and deionized water, stratiform nickel-ferric spinel (NiFe-LDH) is loaded in the matrix and duct of porous graphite phase carbon nitride.The catalyst shows stable and superior catalytic activity in activation persulfate oxidation degradation of methylene blue.
Description
Technical field
The invention belongs to nano material preparation technology and environment protection fields, and in particular to a kind of having for mixed metal load follows
The application in novel composite nano catalyst and its degradation of methylene blue that ring utilizes.
Background technique
Dye industry is the important support industry of Chinese national economy at present, is mainly used for coating, medicine, textile, change
The fields such as cosmetic.But in the production and use process of dyestuff, waste water from dyestuff is unprocessed or not up to discharge standard is directly arranged
Problem of environmental pollution caused by putting is urgently to be resolved.Waste water from dyestuff refers to the waste water given off during producing dyestuff, pigment, tool
Have organic concentration is high, coloration is big, hard-degraded substance is more, complicated components, it is toxic the features such as.Many industry largely use dyestuff,
Inevitable discharge largely has intermittent and unstable water quality waste water from dyestuff simultaneously, thus difficulty is handled.
Contain basic group in the structure of the dye of positive ion (basic dye), color is rich and gaudy, good water solubility, contains complexity
Aromatic group thus be difficult to remove coloration, become the problem of dye wastewater treatment.Therefore, efficient process waste water from dyestuff is found
Technical method becomes the hot spot studied both at home and abroad.
Metal nanoparticle is faced with serious stability problem in actual application, current effective method
Exactly metal nanoparticle is supported on various solid phase carriers to protect them from reuniting and influence.Graphite phase carbon nitride (g-
C3N4) have the advantages that special electro-optic structure and high chemical and thermal stability, but specific surface area is not big enough, quantum
Low efficiency.And nano lamellar hydrotalcite has many advantages, such as that good biocompatibility, ion exchange capacity are big, surface area is big just can be with
It compensates its defect.
Summary of the invention
The object of the present invention is to provide a kind of advanced composite material (ACM)s and preparation method thereof of catalytic degradation methylene blue, and will
In its reaction for being applied to catalytic degradation methylene blue, preparation method is rationally simple, and catalytic oxidation performance is stablized, catalysis oxidation
High efficiency.
The present invention is condensed to form porous graphite phase carbon nitride using high temperature sintering, so using acid processing graphite phase carbon nitride
Ultrasonic disperse is utilized in the solution of metal salt configuration afterwards, in conjunction with confinement growing principle, by nano lamellar nickel-ferric spinel
(NiFe-LDH) duct and surface for loading to porous graphite phase carbon nitride finally obtained good dispersion load nano lamellar nickel
Molten iron talcum has the NEW TYPE OF COMPOSITE function nano catalyst recycled.
To achieve the above object, the technical solution that this discovery uses are as follows:
A kind of support type graphite phase carbon nitride composite material, the composite material are that nano lamellar nickel-ferric spinel loads graphite
Phase carbon nitride.
The preparation of the NEW TYPE OF COMPOSITE function nano catalyst with circulation catalysis of supported mixed metal of the present invention
Method includes several steps:
(1) it by urea grind into powder, pours into alumina crucible with cover, is put into 80 DEG C of baking ovens dry 4h.Muffle
Furnace temperature sets 550 DEG C, calcination 2h, 5 DEG C/min of heating rate.Be cooled to room temperature taking-up to in-furnace temperature, with dehydrated alcohol and
Deionized water is washed for several times repeatedly, is ground after dry, is obtained the porous graphite phase carbon nitride of pale yellow powder shape (g-C3N4).
(2) by deionization is added in graphite phase carbon nitride powder obtained after dehydrated alcohol washing is dry in step (1)
After water, the Fe (NO of molar ratio 4: 1 is added3)3·9H2O and Ni (NO3)2·6H2O forms solution A, subsequent ultrasonic disperse 10min.
(3) 40mL deionized water is separately taken, 40mmol sodium hydroxide is added and 4mmol sodium carbonate forms solution B.B is slow
It instills in A, is centrifuged after being vigorously stirred 4h, sediment is washed with deionized for several times to neutral.60 DEG C of dry 12h are up to stratiform nickel
Molten iron talcum loads graphite phase carbon nitride composite material.
The present invention also provides it is a kind of by above-mentioned support type graphite phase carbon nitride composite material degradation of methylene blue application.
Specific steps include the following: that support type graphite phase carbon nitride composite material is added to concentration in the ratio of 1.0g/L~1.5g/L
In solution for the methylene blue of 10mg/L, sodium peroxydisulfate is added, reaction carries out under conditions of natural light or dark, reaction temperature
Degree is room temperature, and whole methylene blue degradations can be completed in reaction time 60min.
Application method described in above-mentioned steps, sodium peroxydisulfate and methylene blue molar ratio are 20: 1.
Detailed description of the invention
Fig. 1: for the X-ray diffractogram of the advanced composite material (ACM) of load Ni/Fe made from embodiment 2.
Fig. 2: for the x-ray photoelectron spectroscopy figure of the advanced composite material (ACM) of load Ni/Fe made from embodiment 2
Fig. 3: for the scanning electron microscope (SEM) photograph of the advanced composite material (ACM) of load Ni/Fe made from embodiment 2
Fig. 4: for the transmission electron microscope picture of the advanced composite material (ACM) of load Ni/Fe made from embodiment 2
Specific embodiment
Below with reference to specific implementation case, the present invention is further explained, it should be understood that these embodiments are merely to illustrate this hair
Bright rather than limit the scope of the invention, after the present invention has been read, those skilled in the art are to of the invention various etc.
The modification of valence form falls within the application range as defined in the appended claims.
Embodiment 1
1) it by 10g urea grind into powder, pours into alumina crucible with cover, is put into 80 DEG C of baking ovens dry 4h, obtains
Powders A.
2) above-mentioned powders A is placed in Muffle furnace, temperature sets 550 DEG C, calcination 2h, 5 DEG C/min of heating rate.To warm in furnace
Degree is cooled to room temperature taking-up, obtains powder B.
3) powder B dehydrated alcohol and deionized water are washed for several times repeatedly, is ground after dry, obtains pale yellow powder shape stone
Black phase carbon nitride.
Embodiment 2
1) it by 10g urea grind into powder, pours into alumina crucible with cover, is put into 80 DEG C of baking ovens dry 4h, obtains
Powders A.
2) above-mentioned powders A is placed in Muffle furnace, temperature sets 550 DEG C, calcination 2h, 5 DEG C/min of heating rate.To warm in furnace
Degree is cooled to room temperature taking-up, obtains powder B.
3) powder B dehydrated alcohol and deionized water are washed for several times repeatedly, is ground after dry, it is more obtains pale yellow powder shape
Hole graphite phase carbon nitride g-C3N4。
4) Fe (NO of molar ratio 4: 1 is added in 40mL deionized water3)3·9H2O and Ni (NO3)2·6H2O forms solution
A。
5) a certain amount of porous graphite phase carbon nitride g-C is added thereto3N4, subsequent ultrasonic disperse 10min.
6) 40mL deionized water is separately taken, 40mmol sodium hydroxide is added and 4mmol sodium carbonate forms solution B.
7) solution B is slowly dropped into solution A, is centrifuged after being vigorously stirred 4h, sediment is washed with deionized for several times extremely
It is neutral.60 DEG C of dry 12h can obtain stratiform nickel-ferric spinel load graphite phase carbon nitride composite material g-C3N4@NiFe-LDH。
The X-ray diffraction picture of stratiform nickel-ferric spinel (NiFe-LDH) the load graphite phase carbon nitride composite material of above-mentioned preparation
As shown in Figure 1, from the figure, it can be seen that g-C3N4@NiFe-LDH sample has apparent characteristic diffraction peak.Characteristic peak respectively corresponds
In g-C3N4, NiFe-LDH crystal face, both show successfully to be combined with each other.
The x-ray photoelectron spectroscopy picture of the stratiform nickel-ferric spinel load graphite phase carbon nitride composite material of above-mentioned preparation
As shown in Figure 2, it was demonstrated that NiFe-LDH is successfully supported on g-C3N4On.
Scanning electron microscopic picture such as Fig. 3 institute of the stratiform nickel-ferric spinel load graphite phase carbon nitride composite material of above-mentioned preparation
Show, it can be seen that NiFe-LDH is covered on g-C3N4On, and the two is well combined.
Transmission electron microscope picture such as Fig. 4 institute of the stratiform nickel-ferric spinel load graphite phase carbon nitride composite material of above-mentioned preparation
Show, it can be seen that the substance after compound still has laminar structured, g-C3N4It is remained unchanged with the basic pattern of NiFe-LDH.
Embodiment 3
1) support type graphite phase carbon nitride composite material is added to concentration in the ratio of 1.0g/L~1.5g/L is 10mg/
In the solution of the methylene blue of L,
2) sodium peroxydisulfate and methylene blue molar ratio are 20: 1.Sodium peroxydisulfate is added, reacts the item in natural light or dark
It is carried out under part, reaction temperature is room temperature, and whole methylene blue degradations can be completed in reaction time 60min.
The novel material that meets of above-mentioned preparation carries out degradation application to methylene blue, g-C3N4Activate persulfate
120min degradation rate reaches 93.8%, NiFe-LDH activation persulfate 120min degradation rate and reaches 71.3%, and g-C3N4@
NiFe-LDH activates persulfate, and only 60min degradation rate just reaches 99.7%, it is seen that g-C3N4@NiFe-LDH activates persulfate
Degradation of methylene blue significant effect.
Claims (9)
1. a kind of support type graphite phase carbon nitride composite material, which is characterized in that the composite material is stratiform nickel-ferric spinel
(NiFe-LDH) load graphite phase carbon nitride: the graphite phase carbon nitride be porous structure, pore size 50m-100m, than
Surface area is 10m2/ g~80m2/ g, Ni-Fe homoepitaxial are in the surface and duct of graphite phase carbon nitride.
2. support type graphite phase carbon nitride composite material described in claim 1, which is characterized in that Fe, Ni are carried on stone simultaneously
Black phase carbon nitride.
3. the preparation method of any one of the claim 1-2 support type graphite phase carbon nitride composite material, which is characterized in that packet
Include following steps:
(1) it by urea grind into powder, pours into alumina crucible with cover, is put into 80 DEG C of baking ovens dry 4h.Muffle furnace temperature
550 DEG C, calcination 2h of degree setting, 5 DEG C/min of heating rate.Be cooled to room temperature taking-up to in-furnace temperature, with dehydrated alcohol and go from
Sub- water washs for several times repeatedly, grinds after dry, obtains the porous graphite phase carbon nitride (g-C of pale yellow powder shape3N4)。
(2) by after deionized water is added in graphite phase carbon nitride powder obtained after dehydrated alcohol washing is dry in step (1),
Fe (the NO of molar ratio 4: 1 is added3)3·9H2O and Ni (NO3)2·6H2O forms solution A, subsequent ultrasonic disperse 10min.
(3) 40mL deionized water is separately taken, 40mmol sodium hydroxide is added and 4mmol sodium carbonate forms solution B.B is slowly dropped into A
In, it is centrifuged after being vigorously stirred 4h, sediment is washed with deionized for several times to neutral.60 DEG C of dry 12h are negative up to Ni-Fe joint
Carry graphite phase carbon nitride composite material.
4. the preparation method of support type graphite phase carbon nitride composite material described in claim 3, which is characterized in that in step (1),
550 DEG C are warming up to the heating rate of 5 DEG C/min, the straight room temperature of natural cooling finally obtains the porous graphite-phase of yellow flake
Carbonitride (mpg-C3N4) powder
5. the preparation method of support type graphite phase carbon nitride composite material described in claim 3, which is characterized in that in step (2),
Obtained porous graphite phase carbon nitride powder is added in dehydrated alcohol and deionized water mixed solution, molar ratio 4 is added:
1 Fe (NO3)3·9H2O and Ni (NO3)2·6H2O solution A.
6. the preparation method of support type graphite phase carbon nitride composite material described in claim 3, which is characterized in that step (3) is another
40mL deionized water is taken, 40mmol sodium hydroxide is added and 4mmol sodium carbonate forms solution B.B is slowly dropped into A, is acutely stirred
It is centrifuged after mixing 4h, sediment is washed with deionized for several times to neutral.60 DEG C of dry 12h can obtain (NiFe-LDH) load graphite-phase
Nitrogenize carbon composite.
7. claim 1-6 appoints application of the item support type graphite phase carbon nitride composite material on degradation of methylene blue.
8. application as claimed in claim 7, it is characterised in that specific steps include the following: that support type graphite phase carbon nitride is compound
Material is added in the solution for the methylene blue that concentration is 10mg/L in the ratio of 1.0g/L~1.5g/L, and sodium peroxydisulfate is added,
Reaction carries out under conditions of natural light or dark, and reaction temperature is room temperature, and reaction time 60min can be completed whole
Methylene blue degradation.
9. application according to any one of claims 8, which is characterized in that sodium peroxydisulfate is 20: 1 with methylene blue molar ratio.
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