CN105879894B - One kind (NH4)2SiF6/mpg-C3N4Powder and its preparation method and application - Google Patents
One kind (NH4)2SiF6/mpg-C3N4Powder and its preparation method and application Download PDFInfo
- Publication number
- CN105879894B CN105879894B CN201610261128.2A CN201610261128A CN105879894B CN 105879894 B CN105879894 B CN 105879894B CN 201610261128 A CN201610261128 A CN 201610261128A CN 105879894 B CN105879894 B CN 105879894B
- Authority
- CN
- China
- Prior art keywords
- mpg
- sif
- powder
- mixed liquor
- value
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Active
Links
- 229910019975 (NH4)2SiF6 Inorganic materials 0.000 title claims abstract description 57
- 238000002360 preparation method Methods 0.000 title abstract description 7
- 239000000843 powder Substances 0.000 claims abstract description 112
- 229910004074 SiF6 Inorganic materials 0.000 claims abstract description 33
- 238000010438 heat treatment Methods 0.000 claims abstract description 32
- 238000003756 stirring Methods 0.000 claims abstract description 26
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims abstract description 16
- 239000007864 aqueous solution Substances 0.000 claims abstract description 16
- 229920000877 Melamine resin Polymers 0.000 claims abstract description 13
- 230000001699 photocatalysis Effects 0.000 claims abstract description 12
- 229910017665 NH4HF2 Inorganic materials 0.000 claims abstract description 8
- 238000007146 photocatalysis Methods 0.000 claims abstract description 7
- 239000007787 solid Substances 0.000 claims description 20
- 238000005516 engineering process Methods 0.000 claims description 13
- 239000002904 solvent Substances 0.000 claims description 13
- 238000004519 manufacturing process Methods 0.000 claims description 11
- 238000001354 calcination Methods 0.000 claims description 10
- 150000007974 melamines Chemical class 0.000 claims description 10
- 238000006731 degradation reaction Methods 0.000 claims description 7
- 230000015556 catabolic process Effects 0.000 claims description 6
- 238000010792 warming Methods 0.000 claims description 4
- 239000000356 contaminant Substances 0.000 claims description 3
- 239000013335 mesoporous material Substances 0.000 claims description 3
- 239000000377 silicon dioxide Substances 0.000 claims description 3
- 229910052681 coesite Inorganic materials 0.000 claims description 2
- 229910052906 cristobalite Inorganic materials 0.000 claims description 2
- 238000001035 drying Methods 0.000 claims description 2
- 239000000203 mixture Substances 0.000 claims description 2
- 229910052682 stishovite Inorganic materials 0.000 claims description 2
- 229910052905 tridymite Inorganic materials 0.000 claims description 2
- 229910052710 silicon Inorganic materials 0.000 claims 1
- 239000010703 silicon Substances 0.000 claims 1
- 238000000034 method Methods 0.000 abstract description 4
- 238000006243 chemical reaction Methods 0.000 abstract description 3
- JDSHMPZPIAZGSV-UHFFFAOYSA-N melamine Chemical compound NC1=NC(N)=NC(N)=N1 JDSHMPZPIAZGSV-UHFFFAOYSA-N 0.000 abstract description 3
- 230000035484 reaction time Effects 0.000 abstract description 3
- 239000008367 deionised water Substances 0.000 abstract 1
- 229910021641 deionized water Inorganic materials 0.000 abstract 1
- 238000003786 synthesis reaction Methods 0.000 abstract 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 abstract 1
- 239000002245 particle Substances 0.000 description 8
- PYWVYCXTNDRMGF-UHFFFAOYSA-N rhodamine B Chemical compound [Cl-].C=12C=CC(=[N+](CC)CC)C=C2OC2=CC(N(CC)CC)=CC=C2C=1C1=CC=CC=C1C(O)=O PYWVYCXTNDRMGF-UHFFFAOYSA-N 0.000 description 4
- 229940043267 rhodamine b Drugs 0.000 description 4
- 239000013078 crystal Substances 0.000 description 3
- 230000000593 degrading effect Effects 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- 230000001276 controlling effect Effects 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 238000009826 distribution Methods 0.000 description 2
- 239000010410 layer Substances 0.000 description 2
- 239000007788 liquid Substances 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 239000002957 persistent organic pollutant Substances 0.000 description 2
- 239000011148 porous material Substances 0.000 description 2
- 239000004065 semiconductor Substances 0.000 description 2
- 238000005406 washing Methods 0.000 description 2
- QGZKDVFQNNGYKY-UHFFFAOYSA-O Ammonium Chemical compound [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 description 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- YCKRFDGAMUMZLT-UHFFFAOYSA-N Fluorine atom Chemical compound [F] YCKRFDGAMUMZLT-UHFFFAOYSA-N 0.000 description 1
- 238000005411 Van der Waals force Methods 0.000 description 1
- 125000003118 aryl group Chemical group 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 230000002708 enhancing effect Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 229910052731 fluorine Inorganic materials 0.000 description 1
- 239000011737 fluorine Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- 239000011229 interlayer Substances 0.000 description 1
- 238000011068 loading method Methods 0.000 description 1
- 239000008204 material by function Substances 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- 230000003287 optical effect Effects 0.000 description 1
- 239000011941 photocatalyst Substances 0.000 description 1
- 238000013033 photocatalytic degradation reaction Methods 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 238000005215 recombination Methods 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 238000002336 sorption--desorption measurement Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 239000002351 wastewater Substances 0.000 description 1
- 238000004804 winding Methods 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
-
- A—HUMAN NECESSITIES
- A62—LIFE-SAVING; FIRE-FIGHTING
- A62D—CHEMICAL MEANS FOR EXTINGUISHING FIRES OR FOR COMBATING OR PROTECTING AGAINST HARMFUL CHEMICAL AGENTS; CHEMICAL MATERIALS FOR USE IN BREATHING APPARATUS
- A62D3/00—Processes for making harmful chemical substances harmless or less harmful, by effecting a chemical change in the substances
- A62D3/10—Processes for making harmful chemical substances harmless or less harmful, by effecting a chemical change in the substances by subjecting to electric or wave energy or particle or ionizing radiation
- A62D3/17—Processes for making harmful chemical substances harmless or less harmful, by effecting a chemical change in the substances by subjecting to electric or wave energy or particle or ionizing radiation to electromagnetic radiation, e.g. emitted by a laser
- A62D3/176—Ultraviolet radiations, i.e. radiation having a wavelength of about 3nm to 400nm
-
- B01J35/39—
-
- B01J35/615—
-
- B01J35/647—
-
- 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
- C02F1/32—Treatment of water, waste water, or sewage by irradiation with ultraviolet light
-
- A—HUMAN NECESSITIES
- A62—LIFE-SAVING; FIRE-FIGHTING
- A62D—CHEMICAL MEANS FOR EXTINGUISHING FIRES OR FOR COMBATING OR PROTECTING AGAINST HARMFUL CHEMICAL AGENTS; CHEMICAL MATERIALS FOR USE IN BREATHING APPARATUS
- A62D2101/00—Harmful chemical substances made harmless, or less harmful, by effecting chemical change
- A62D2101/20—Organic substances
-
- 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
-
- 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
Abstract
The invention discloses one kind (NH4)2SiF6/mpg‑C3N4Powder and its preparation method and application, melamine is mixed with Ludox, and heating stirring obtains white powder, yellow powder is obtained after white powder is calcined to doing, and yellow powder is added NH4HF2In aqueous solution, stirring removes the SiO in yellow powder2, mixed liquor is formed, 6~24h is washed to mixed liquor with deionized water, the pH value for controlling mixed liquor is 2.5~7.0, then dries, that is, obtains (NH4)2SiF6/mpg‑C3N4Powder.Flow of the present invention is simple, and operation is easy, and the reaction time is shorter, and reaction condition is gentle, (the NH of synthesis4)2SiF6/mpg‑C3N4Powder has higher photocatalytic activity, there is provided one improves mpg C3N4Photocatalysis efficiency feasible method, have a good application prospect.
Description
Technical field
The invention belongs to field of functional materials, and in particular to one kind (NH4)2SiF6/mpg-C3N4Powder and preparation method thereof
And application.
Background technology
With the deterioration of environment, Green Chemistry becomes the inevitable requirement of human social.Semiconductor is because of it
Can directly it be widely studied using sunlight.mpg-C3N4Semiconductor illustrates very high light in terms of degradable organic pollutant
Catalytic activity, it has the layer structure similar to graphite, is stacked between layers by Van der Waals force interaction,
Its band gap only has 2.7eV, and good optical property and excellent stability cause it to have wide answer in field of photocatalytic material
Use prospect.But electronics-hole-recombination rate is excessive so that mpg-C3N4Photocatalytic activity reduces.By doping, compound, surface is photosensitive
The means such as change, noble metal loading have many reports to improve its photocatalytic activity.
At present, in terms of photocatalyst for degrading pollutant, (NH4)2SiF6/mpg-C3N4Powder possesses the work of photocatalytic activity
There is not been reported for work, also without patent and document report mistake.
The content of the invention
It is an object of the invention to provide one kind (NH4)2SiF6/mpg-C3N4Powder and its preparation method and application, the party
Method is easy to operate, and the reaction time is short, and reaction condition is gentle, (the NH of preparation4)2SiF6/mpg-C3N4The specific surface area of powder is significantly
Increase, and there is higher degrading activity under ultraviolet light.
To reach above-mentioned purpose, the present invention uses following technical scheme：
One kind (NH4)2SiF6/mpg-C3N4Raw powder's production technology, comprises the following steps：
Step 1：A g melamines are uniformly mixed with B mL Ludox, heating stirring to solvent is evaporated, and it is solid to obtain white
Body, wherein A:B=(48~52):(190~210)；
Step 2：By white solid it is finely ground after is fitted into crucible, be warming up to 540~560 DEG C, calcining 4h, obtains yellow powder
Body；
Step 3：Yellow powder is added to NH4HF2In aqueous solution, stirring removes the SiO in yellow powder2, mixed
Liquid；
Step 4：Mixed liquor is washed with deionized, wash time is 6~24h, and control the pH value of mixed liquor for 2.5~
7.0, then mixed liquor is dried, that is, obtains (NH4)2SiF6/mpg-C3N4Powder.
Contain the SiO that mass fraction is 28~32% in the Ludox2, and SiO2Average grain diameter be 10~14nm.
Heating-up temperature when heating stirring to solvent is evaporated in the step 1 is 85~95 DEG C.
Heating rate when heating up in the step 2 is 2~3 DEG C/min.
C g yellow powders are added to D mL NH in the step 34HF2In aqueous solution, C:D=(8~12):(350~
450), NH4HF2The concentration of aqueous solution is 3.5~4.5mol/L.
When wash time in the step 4 is 6h, the pH value for controlling mixed liquor is 2.5；When wash time is 12h, control
The pH value of mixed liquor processed is 4.3；When wash time is 18h, the pH value for controlling mixed liquor is 5.1；When wash time is 24h, control
The pH value of mixed liquor processed is 7.0.
Drying in the step 4 is dry 10~12h at 75~85 DEG C.
(the NH4)2SiF6/mpg-C3N4(NH made from raw powder's production technology4)2SiF6/mpg-C3N4Powder, should
(NH4)2SiF6/mpg-C3N4Powder is mesoporous material, is mpg-C3N4(NH4)2SiF6Mixture, wherein mpg-C3N4Matter
Amount fraction is x, (NH4)2SiF6Mass fraction be ＜ y≤47.61% of y, 52.39%≤x ＜ 100%, 0, and (NH4)2SiF6
Crystal form be Emission in Cubic, space structure group is Fm-3m.
When the wash time in step 4 is 6h, the pH value of mixed liquor is 2.5, obtained (NH4)2SiF6/mpg-C3N4Powder
The aperture of body is 5~50nm, specific surface area 209.49m2/ g, x=52.39%, y=47.61%；When the washing in step 4
When time is 12h, the pH value of mixed liquor is 4.3, obtained (NH4)2SiF6/mpg-C3N4The aperture of powder is 5~50nm, than
Surface area is 158.20m2/ g, x=92.90%, y=7.10%；When the pH value that the wash time in step 4 is 18h, mixed liquor
For 5.1 when, obtained (NH4)2SiF6/mpg-C3N4The aperture of powder is 5~20nm, specific surface area 131.52m2/ g, x=
99.24%, y=0.76%.
(the NH4)2SiF6/mpg-C3N4The powder application in terms of photocatalysis degradation organic contaminant under ultraviolet light.
Compared to existing technology, beneficial effects of the present invention are：
(NH provided by the invention4)2SiF6/mpg-C3N4Raw powder's production technology, using melamine as nitrogen source, with NH4HF2
For source of ammonium and Fluorine source, using silica as template, first melamine is mixed with Ludox, heating stirring to solvent is evaporated,
White powder is obtained, then calcines white powder to obtain yellow powder, then yellow powder is added NH4HF2In aqueous solution, stirring
Remove the SiO in yellow powder2, mixed liquor is formed, mixed liquor is finally washed with deionized, and the pH value of mixed liquor is controlled,
Then dry, that is, obtain (NH4)2SiF6/mpg-C3N4Powder.This method flow is simple, and operation is easy, and the reaction time is shorter, instead
Answer mild condition, obtained (NH4)2SiF6/mpg-C3N4The mpg-C of powder and pure phase3N4Powder is compared, and specific surface area increases
Greatly, and there is higher photocatalytic activity under ultraviolet light.The present invention is mixed by the regulation and control to washing time length and control
The pH value of liquid is closed, (NH can be regulated and controled in product4)2SiF6And mpg-C3N4Content and product aperture and specific surface area, system
It is standby to have gone out there is (the NH of bigger serface4)2SiF6/mpg-C3N4Powder, and under ultraviolet light, (NH4)2SiF6/mpg-
C3N4Powder has the ability of high degradable organic pollutant, and degradation efficiency is compared with mpg-C3N4Increase, can be in photocatalytic degradation
It is applied in terms of organic pollution.In addition, in photocatalysis field, (NH4)2SiF6It is a kind of and what is had not been reported has
The novel substance of photocatalytic activity.The present invention provides one kind to improve mpg-C3N4Photocatalysis efficiency feasible method, and for the first time
Propose (NH4)2SiF6This material has a good application prospect in the application of photocatalysis field.
Brief description of the drawings
Fig. 1 is that the present invention prepares (NH4)2SiF6/mpg-C3N4The XRD diagram of powder；
Fig. 2 is that the present invention prepares (NH4)2SiF6/mpg-C3N4The XRD refine figures of powder；
Fig. 3 is that the present invention prepares (NH4)2SiF6/mpg-C3N4The N of powder2Adsorption-desorption curve；
Fig. 4 is that the present invention prepares (NH4)2SiF6/mpg-C3N4The graph of pore diameter distribution of powder；
Fig. 5 is that the present invention prepares (NH4)2SiF6/mpg-C3N4Degradation rate-time of degraded RhB is bent under powder ultraviolet light
Line chart.
Embodiment
The present invention is described in further details with reference to the present invention preferably embodiment and attached drawing.
Embodiment 1：
Step 1：By 50g melamines and 200mL Ludox (containing the SiO that mass fraction is 30%2, particle diameter 12nm) and it is mixed
Close uniformly, heating stirring to solvent is evaporated at 90 DEG C, obtains white solid；
Step 2：By white solid it is finely ground after is fitted into crucible, with the heating of the heating rate of 2.5 DEG C/min in Muffle furnace
To 550 DEG C of calcining 4h, yellow powder is obtained；
Step 3：10g yellow powders are added to the NH that 400mL concentration is 4mol/L4HF2In aqueous solution, long-time magnetic force
Stirring, removes the SiO in yellow powder2, obtain mixed liquor；
Step 4：Mixed liquor, wash time 18h is washed with deionized, and control mixed liquor pH value be 5.1, then
Mixed liquor is dried into 10h at 80 DEG C, that is, obtains (NH4)2SiF6/mpg-C3N4Powder.
Embodiment 2：
Step 1：By 50g melamines and 200mL Ludox (containing the SiO that mass fraction is 30%2, particle diameter 12nm) and it is mixed
Close uniformly, heating stirring to solvent is evaporated at 90 DEG C, obtains white solid；
Step 2：By white solid it is finely ground after is fitted into crucible, with the heating of the heating rate of 2.5 DEG C/min in Muffle furnace
To 550 DEG C of calcining 4h, yellow powder is obtained；
Step 3：10g yellow powders are added to the NH that 400mL concentration is 4mol/L4HF2In aqueous solution, long-time magnetic force
Stirring, removes the SiO in yellow powder2, obtain mixed liquor；
Step 4：Mixed liquor, wash time 12h is washed with deionized, and control mixed liquor pH value be 4.3, then
Mixed liquor is dried into 10h at 80 DEG C, that is, obtains (NH4)2SiF6/mpg-C3N4Powder.
Embodiment 3：
Step 1：By 50g melamines and 200mL Ludox (containing the SiO that mass fraction is 30%2, particle diameter 12nm) and it is mixed
Close uniformly, heating stirring to solvent is evaporated at 90 DEG C, obtains white solid；
Step 2：By white solid it is finely ground after is fitted into crucible, with the heating of the heating rate of 2.5 DEG C/min in Muffle furnace
To 550 DEG C of calcining 4h, yellow powder is obtained；
Step 3：10g yellow powders are added to the NH that 400mL concentration is 4mol/L4HF2In aqueous solution, long-time magnetic force
Stirring, removes the SiO in yellow powder2, obtain mixed liquor；
Step 4：Mixed liquor, wash time 6h is washed with deionized, and control mixed liquor pH value be 2.5, then
Mixed liquor is dried into 10h at 80 DEG C, that is, obtains (NH4)2SiF6/mpg-C3N4Powder.
Embodiment 4：
Step 1：By 50g melamines and 200mL Ludox (containing the SiO that mass fraction is 30%2, particle diameter 12nm) and it is mixed
Close uniformly, heating stirring to solvent is evaporated at 90 DEG C, obtains white solid；
Step 2：By white solid it is finely ground after is fitted into crucible, with the heating of the heating rate of 2.5 DEG C/min in Muffle furnace
To 550 DEG C of calcining 4h, yellow powder is obtained；
Step 3：10g yellow powders are added to the NH that 400mL concentration is 4mol/L4HF2In aqueous solution, long-time magnetic force
Stirring, removes the SiO in yellow powder2, obtain mixed liquor；
Step 4：Mixed liquor, wash time 24h is washed with deionized, and control mixed liquor pH value be 7.0, then
Mixed liquor is dried into 10h at 80 DEG C, that is, obtains mpg-C3N4Powder is (without (NH under the conditions of this4)2SiF6Generation, product are pure
mpg-C3N4)。
Embodiment 5：
Step 1：By 48g melamines and 190mL Ludox (containing the SiO that mass fraction is 28%2, particle diameter 10nm) and it is mixed
Close uniformly, heating stirring to solvent is evaporated at 85 DEG C, obtains white solid；
Step 2：By white solid it is finely ground after be fitted into crucible, be warming up in Muffle furnace with the heating rate of 2 DEG C/min
540 DEG C of calcining 4h, obtain yellow powder；
Step 3：8g yellow powders are added to the NH that 350mL concentration is 3.5mol/L4HF2In aqueous solution, long-time magnetic force
Stirring, removes the SiO in yellow powder2, obtain mixed liquor；
Step 4：Mixed liquor, wash time 8h is washed with deionized, and control mixed liquor pH value be 3.1, then
Mixed liquor is dried into 12h at 75 DEG C, that is, obtains (NH4)2SiF6/mpg-C3N4Powder.
Embodiment 6：
Step 1：By 49g melamines and 195mL Ludox (containing the SiO that mass fraction is 29%2, particle diameter 11nm) and it is mixed
Close uniformly, heating stirring to solvent is evaporated at 88 DEG C, obtains white solid；
Step 2：By white solid it is finely ground after be fitted into crucible, be warming up in Muffle furnace with the heating rate of 3 DEG C/min
545 DEG C of calcining 4h, obtain yellow powder；
Step 3：9g yellow powders are added to the NH that 380mL concentration is 3.8mol/L4HF2In aqueous solution, long-time magnetic force
Stirring, removes the SiO in yellow powder2, obtain mixed liquor；
Step 4：Mixed liquor, wash time 15h is washed with deionized, and control mixed liquor pH value be 4.7, then
Mixed liquor is dried into 11.5h at 78 DEG C, that is, obtains (NH4)2SiF6/mpg-C3N4Powder.
Embodiment 7：
Step 1：By 51g melamines and 205mL Ludox (containing the SiO that mass fraction is 31%2, particle diameter 13nm) and it is mixed
Close uniformly, heating stirring to solvent is evaporated at 92 DEG C, obtains white solid；
Step 2：By white solid it is finely ground after is fitted into crucible, with the heating of the heating rate of 2.2 DEG C/min in Muffle furnace
To 555 DEG C of calcining 4h, yellow powder is obtained；
Step 3：11g yellow powders are added to the NH that 420mL concentration is 4.2mol/L4HF2In aqueous solution, long-time magnetic
Power stirs, and removes the SiO in yellow powder2, obtain mixed liquor；
Step 4：Mixed liquor, wash time 21h is washed with deionized, and control mixed liquor pH value be 6.0, then
Mixed liquor is dried into 11h at 82 DEG C, that is, obtains (NH4)2SiF6/mpg-C3N4Powder.
Embodiment 8：
Step 1：By 52g melamines and 210mL Ludox (containing the SiO that mass fraction is 32%2, particle diameter 14nm) and it is mixed
Close uniformly, heating stirring to solvent is evaporated at 95 DEG C, obtains white solid；
Step 2：By white solid it is finely ground after is fitted into crucible, with the heating of the heating rate of 2.8 DEG C/min in Muffle furnace
To 560 DEG C of calcining 4h, yellow powder is obtained；
Step 3：12g yellow powders are added to the NH that 450mL concentration is 4.5mol/L4HF2In aqueous solution, long-time magnetic
Power stirs, and removes the SiO in yellow powder2, obtain mixed liquor；
Step 4：Mixed liquor, wash time 10h is washed with deionized, and control mixed liquor pH value be 3.7, then
Mixed liquor is dried into 10.5h at 85 DEG C, that is, obtains (NH4)2SiF6/mpg-C3N4Powder.
Fig. 1 and Fig. 2 is that the embodiment of the present invention 1~3 prepares (NH respectively4)2SiF6/mpg-C3N4The XRD diagram and XRD of powder
Refine figure, from figure 1 it appears that all obtained (NH4)2SiF6/mpg-C3N4Powder has obvious wide suction at 27.4 °
Peak is received, it belongs to mpg-C3N4(002) crystal face peak, be mpg-C3N4The interlayer stacking peak of middle aromatic rings, shows obtained
(NH4)2SiF6/mpg-C3N4Contain mpg-C in powder3N4.All obtained (NH4)2SiF6/mpg-C3N4Powder 18.3 °,
21.2 °, 37.1 °, 43.2 ° etc. of diffraction maximum correspondence (NH4)2SiF6(111) of (JCDPS No.72-1759), (200),
(222), the crystal face such as (400), shows obtained (NH4)2SiF6/mpg-C3N4(NH in powder4)2SiF6For Emission in Cubic, space
Structure group is Fm-3m.(NH made from embodiment 1 can be calculated by Fig. 24)2SiF6/mpg-C3N4Mpg-C in powder3N4's
Mass fraction is 99.24%, (NH4)2SiF6Mass fraction be 0.76%；(NH made from embodiment 24)2SiF6/mpg-C3N4
Mpg-C in powder3N4Mass fraction be 92.90%, (NH4)2SiF6Mass fraction be 7.10%；Made from embodiment 3
(NH4)2SiF6/mpg-C3N4Mpg-C in powder3N4Mass fraction be 52.39%, (NH4)2SiF6Mass fraction be
47.61%；(NH made from embodiment 44)2SiF6/mpg-C3N4Mpg-C in powder3N4Mass fraction be 100%, (NH4)2SiF6Mass fraction be 0%.With acid enhancing, (NH4)2SiF6Content increase to 47.61% by 0.76%, explanation
Acid condition is conducive to (NH4)2SiF6Generation.
Fig. 3 and Fig. 4 is that the embodiment of the present invention 1~3 prepares (NH respectively4)2SiF6/mpg-C3N4The N of powder2Absorption-de-
Attached isothermal curve figure and graph of pore diameter distribution.From figure 3, it can be seen that (NH made from embodiment 1~34)2SiF6/mpg-C3N4Powder
There are H3 hysteresis winding in body, illustrates (the NH prepared4)2SiF6/mpg-C3N4Powder is mesoporous material.Can be with from Fig. 4
Find out, (NH made from embodiment 14)2SiF6/mpg-C3N4The aperture of powder is smaller, is largely distributed in 5~20nm, compares surface
Product is 131.52m2/ g, (NH made from embodiment 2 and 34)2SiF6/mpg-C3N4The aperture of powder is largely distributed in 5~
50nm, aperture become larger, and specific surface area is respectively 158.20m2/ g, 209.49m2/g。
Fig. 5 is that the embodiment of the present invention 1~3 prepares (NH4)2SiF6/mpg-C3N4The degradation rate of powder rhodamine B degradation-
Time graph.From figure 5 it can be seen that (NH prepared by the present invention4)2SiF6/mpg-C3N4Powder all there is higher degraded to live
Property, the wherein (NH of the preparation of embodiment 34)2SiF6/mpg-C3N4The degrading activity highest of powder is right after ultraviolet light 8min
The degradation rate of rhodamine B (RhB) reaches 90% or so, this explanation (NH4)2SiF6/mpg-C3N4In (NH4)2SiF6Can be effective
Improve (NH in ground4)2SiF6/mpg-C3N4The photocatalytic activity of powder.(NH prepared by the present invention4)2SiF6/mpg-C3N4Powder exists
There is potential application value in terms of environmental wastewater processing and photocatalysis degradation organic contaminant.
The foregoing is merely one embodiment of the present invention, is not all of or unique embodiment, this area are common
Technical staff is the present invention by reading description of the invention any equivalent conversion for taking technical solution of the present invention
Claim covered.
Claims (10)
1. one kind (NH4)2SiF6/mpg-C3N4Raw powder's production technology, it is characterised in that comprise the following steps：
Step 1：A g melamines are uniformly mixed with B mL Ludox, heating stirring to solvent is evaporated, and obtains white solid,
Wherein A:B=(48~52):(190~210)；
Step 2：By white solid it is finely ground after is fitted into crucible, be warming up to 540~560 DEG C, calcining 4h, obtains yellow powder；
Step 3：Yellow powder is added to NH4HF2In aqueous solution, stirring removes the SiO in yellow powder2, obtain mixed liquor；
Step 4：Mixed liquor is washed with deionized, wash time is 6~21h, and control mixed liquor pH value be 2.5~6.0,
Then mixed liquor is dried, that is, obtains (NH4)2SiF6/mpg-C3N4Powder.
2. (NH according to claim 14)2SiF6/mpg-C3N4Raw powder's production technology, it is characterised in that：The silicon
Contain the SiO that mass fraction is 28~32% in colloidal sol2, and SiO2Average grain diameter be 10~14nm.
3. (NH according to claim 14)2SiF6/mpg-C3N4Raw powder's production technology, it is characterised in that：The step 1
Heating-up temperature when middle heating stirring to solvent is evaporated is 85~95 DEG C.
4. (NH according to claim 14)2SiF6/mpg-C3N4Raw powder's production technology, it is characterised in that：The step 2
Heating rate during middle heating is 2~3 DEG C/min.
5. (NH according to claim 14)2SiF6/mpg-C3N4Raw powder's production technology, it is characterised in that：The step 3
It is middle that C g yellow powders are added to D mL NH4HF2In aqueous solution, C:D=(8~12):(350~450), NH4HF2Aqueous solution
Concentration be 3.5~4.5mol/L.
6. (NH according to claim 14)2SiF6/mpg-C3N4Raw powder's production technology, it is characterised in that：The step 4
In wash time when being 6h, the pH value for controlling mixed liquor is 2.5；Or wash time controls the pH value of mixed liquor when being 12h
For 4.3；Or wash time, when being 18h, the pH value for controlling mixed liquor is 5.1.
7. (NH according to claim 14)2SiF6/mpg-C3N4Raw powder's production technology, it is characterised in that：The step 4
In drying be dry 10~12h at 75~85 DEG C.
8. (the NH in claim 1-7 described in any one4)2SiF6/mpg-C3N4(NH made from raw powder's production technology4)2SiF6/mpg-C3N4Powder, it is characterised in that：Should (NH4)2SiF6/mpg-C3N4Powder is mesoporous material, is mpg-C3N4With
(NH4)2SiF6Mixture, wherein mpg-C3N4Mass fraction be x, (NH4)2SiF6Mass fraction be y, 52.39%≤x
＜ 100%, 0 ＜ y≤47.61%, and (NH4)2SiF6Crystal form be Emission in Cubic, space structure group is Fm-3m.
9. (NH according to claim 84)2SiF6/mpg-C3N4Powder, it is characterised in that：When the wash time in step 4
When pH value for 6h, mixed liquor is 2.5, obtained (NH4)2SiF6/mpg-C3N4The aperture of powder is 5~50nm, specific surface area
For 209.49m2/ g, x=52.39%, y=47.61%；When the wash time in step 4 is 12h, the pH value of mixed liquor is 4.3
When, obtained (NH4)2SiF6/mpg-C3N4The aperture of powder is 5~50nm, specific surface area 158.20m2/ g, x=
92.90%, y=7.10%；When the wash time in step 4 is 18h, the pH value of mixed liquor is 5.1, obtained (NH4)2SiF6/mpg-C3N4The aperture of powder is 5~20nm, specific surface area 131.52m2/ g, x=99.24%, y=0.76%.
10. (the NH described in claim 8 or 94)2SiF6/mpg-C3N4Powder photocatalysis degradation organic contaminant under ultraviolet light
The application of aspect.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201610261128.2A CN105879894B (en) | 2016-04-25 | 2016-04-25 | One kind (NH4)2SiF6/mpg-C3N4Powder and its preparation method and application |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201610261128.2A CN105879894B (en) | 2016-04-25 | 2016-04-25 | One kind (NH4)2SiF6/mpg-C3N4Powder and its preparation method and application |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN105879894A CN105879894A (en) | 2016-08-24 |
| CN105879894B true CN105879894B (en) | 2018-05-11 |
Family
ID=56705288
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN201610261128.2A Active CN105879894B (en) | 2016-04-25 | 2016-04-25 | One kind (NH4)2SiF6/mpg-C3N4Powder and its preparation method and application |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN105879894B (en) |
Families Citing this family (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107649164B (en) * | 2017-10-16 | 2020-12-01 | 陕西科技大学 | g-C3N4-xFx/TiO2Coupling heterojunction photocatalyst and preparation method thereof |
Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103011099A (en) * | 2012-12-12 | 2013-04-03 | 常州大学 | Spherical mesoporous carbon nitride material and preparation method thereof |
| CN104525234A (en) * | 2014-12-17 | 2015-04-22 | 上海交通大学 | Preparation method for graphite-phase carbon nitride photocatalytic material |
| CN104692344A (en) * | 2015-02-15 | 2015-06-10 | 南京工程学院 | Preparation method of mesoporous graphite-phase carbon nitride material |
| CN105271141A (en) * | 2015-11-19 | 2016-01-27 | 南京工程学院 | Method for preparing porous graphite-phase carbon nitride material |
-
2016
- 2016-04-25 CN CN201610261128.2A patent/CN105879894B/en active Active
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103011099A (en) * | 2012-12-12 | 2013-04-03 | 常州大学 | Spherical mesoporous carbon nitride material and preparation method thereof |
| CN104525234A (en) * | 2014-12-17 | 2015-04-22 | 上海交通大学 | Preparation method for graphite-phase carbon nitride photocatalytic material |
| CN104692344A (en) * | 2015-02-15 | 2015-06-10 | 南京工程学院 | Preparation method of mesoporous graphite-phase carbon nitride material |
| CN105271141A (en) * | 2015-11-19 | 2016-01-27 | 南京工程学院 | Method for preparing porous graphite-phase carbon nitride material |
Non-Patent Citations (2)
| Title |
|---|
| "Microporous carbon nitride as an effective solid base catalyst for Knoevenagel condensation reactions";Jie Xu et al.;《Journal of Molecular Catalysis A:Chemical》;20130304;第372卷;第105-113页 * |
| "Solubility of (NH4)2SiF6,K2SiF6 and Na2FiF6 in acidic solution";Jerome Frayret et al.;《Chemical Physics Letters》;20060621;第427卷;第356-364页 * |
Also Published As
| Publication number | Publication date |
|---|---|
| CN105879894A (en) | 2016-08-24 |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| CN102285686B (en) | Method for preparing iron-nitrogen codoped mesoporous nano titanium dioxide by fast sol-gel method | |
| CN105195198B (en) | A kind of mpg-C3N4/Bi0.9Nd0.1VO4Composite photo-catalyst and its preparation method and application | |
| CN105964236A (en) | Preparing method for graphene/titanium dioxide photocatalyst | |
| CN101391811B (en) | Method for preparing high specific surface area titanic oxide | |
| CN102633302B (en) | Method for synthesizing meso pore TiO2 in ionic liquid/water media by cellulose templates | |
| CN103172030A (en) | Oxide powder and preparation method thereof as well as catalyst and carrier thereof | |
| CN107413364B (en) | Preparation method and application of titanium dioxide-coated graphite-phase carbon nitride composite photocatalyst with hollow mesoporous core-shell structure | |
| CN102674451A (en) | Preparation method of {001} face exposed titanium dioxide nanocrystals | |
| CN101293669A (en) | Method for preparing nano-titanium dioxide powder with controllable phase ratio of anatase and rutile | |
| CN103464181A (en) | Preparation method of bismuth oxyhalide/ titanium dioxide composite photocatalyst | |
| CN102515270A (en) | Preparation method of mixed crystal-type nanoscale TiO2 having exposed (001) crystal faces | |
| CN105217676A (en) | There is titania aerogel of nanometer sheet and nano-porous structure and preparation method thereof | |
| CN103691433A (en) | Ag-doped TiO2 material, and preparation method and application thereof | |
| CN102600880A (en) | Preparation method of visible light-response titanium dioxide photocatalytic liquid | |
| CN107008246A (en) | Graphene quantum dot is sensitized the preparation method of sea urchin shape photocatalysis material of titanium dioxide | |
| CN103601253B (en) | Disk type alpha-Fe2O3 photocatalyst and preparation method and application thereof | |
| CN102989444B (en) | Cerium ion doped tungsten trioxide catalyst and preparation method and application thereof | |
| CN104226320B (en) | The preparation method of vanadium boron codope titanium dioxide and nickel oxide composite photo-catalyst | |
| CN104941617A (en) | Titanium dioxide nanosheet grafted titanium dioxide nanorod heterojunction composite material | |
| CN105879894B (en) | One kind (NH4)2SiF6/mpg-C3N4Powder and its preparation method and application | |
| CN103962118A (en) | Preparation method of TiO2 photocatalyst mesh and TiO2 photocatalyst mesh | |
| CN107812532B (en) | g-C3N4/Zn2SnO4-xNxHeterojunction photocatalyst and preparation method thereof | |
| CN105233821A (en) | Strontium-doped and silver-doped nanometer titanium dioxide visible light catalyst | |
| CN109289887B (en) | Preparation method and application of nitrogen and vanadium co-doped titanium dioxide/bismuth tantalate Z-type heterojunction photocatalyst | |
| CN110227458B (en) | Copper-doped mesoporous titanium dioxide composite material and application thereof |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| C06 | Publication | ||
| PB01 | Publication | ||
| C10 | Entry into substantive examination | ||
| SE01 | Entry into force of request for substantive examination | ||
| GR01 | Patent grant | ||
| GR01 | Patent grant |