CN112495436A - Polypyrrole/titanium dioxide/graphite phase carbon nitride ternary composite photocatalytic material and preparation method thereof - Google Patents
Polypyrrole/titanium dioxide/graphite phase carbon nitride ternary composite photocatalytic material and preparation method thereof Download PDFInfo
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- CN112495436A CN112495436A CN202011384942.6A CN202011384942A CN112495436A CN 112495436 A CN112495436 A CN 112495436A CN 202011384942 A CN202011384942 A CN 202011384942A CN 112495436 A CN112495436 A CN 112495436A
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- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 title claims abstract description 92
- JMANVNJQNLATNU-UHFFFAOYSA-N oxalonitrile Chemical compound N#CC#N JMANVNJQNLATNU-UHFFFAOYSA-N 0.000 title claims abstract description 53
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 39
- 229910002804 graphite Inorganic materials 0.000 title claims abstract description 39
- 239000010439 graphite Substances 0.000 title claims abstract description 39
- 229920000128 polypyrrole Polymers 0.000 title claims abstract description 38
- 239000004408 titanium dioxide Substances 0.000 title claims abstract description 37
- 239000011206 ternary composite Substances 0.000 title claims abstract description 30
- 239000000463 material Substances 0.000 title claims abstract description 26
- 230000001699 photocatalysis Effects 0.000 title claims abstract description 26
- 238000002360 preparation method Methods 0.000 title claims abstract description 11
- KAESVJOAVNADME-UHFFFAOYSA-N Pyrrole Chemical compound C=1C=CNC=1 KAESVJOAVNADME-UHFFFAOYSA-N 0.000 claims abstract description 26
- 239000002135 nanosheet Substances 0.000 claims abstract description 15
- 238000000034 method Methods 0.000 claims abstract description 11
- 239000000178 monomer Substances 0.000 claims abstract description 11
- 239000000725 suspension Substances 0.000 claims abstract description 11
- QAOWNCQODCNURD-UHFFFAOYSA-N sulfuric acid Substances OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims abstract description 10
- 239000007864 aqueous solution Substances 0.000 claims abstract description 8
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 8
- 239000005457 ice water Substances 0.000 claims abstract description 7
- 238000011065 in-situ storage Methods 0.000 claims abstract description 6
- 239000007800 oxidant agent Substances 0.000 claims abstract description 6
- 230000001590 oxidative effect Effects 0.000 claims abstract description 6
- 238000006116 polymerization reaction Methods 0.000 claims abstract description 6
- 238000005406 washing Methods 0.000 claims abstract description 6
- 239000002131 composite material Substances 0.000 claims abstract description 5
- 238000003756 stirring Methods 0.000 claims abstract description 5
- 238000001291 vacuum drying Methods 0.000 claims abstract 3
- 238000001914 filtration Methods 0.000 claims abstract 2
- 239000000843 powder Substances 0.000 claims abstract 2
- 239000000243 solution Substances 0.000 claims description 11
- 239000008367 deionised water Substances 0.000 claims description 5
- 229910021641 deionized water Inorganic materials 0.000 claims description 5
- 230000035484 reaction time Effects 0.000 claims description 4
- 229940044631 ferric chloride hexahydrate Drugs 0.000 claims 2
- NQXWGWZJXJUMQB-UHFFFAOYSA-K iron trichloride hexahydrate Chemical compound O.O.O.O.O.O.[Cl-].Cl[Fe+]Cl NQXWGWZJXJUMQB-UHFFFAOYSA-K 0.000 claims 2
- 239000007900 aqueous suspension Substances 0.000 claims 1
- 238000001132 ultrasonic dispersion Methods 0.000 claims 1
- 230000009286 beneficial effect Effects 0.000 abstract description 3
- 238000001035 drying Methods 0.000 abstract description 2
- 239000010865 sewage Substances 0.000 abstract 1
- 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 description 19
- 229960000907 methylthioninium chloride Drugs 0.000 description 19
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 12
- 230000015556 catabolic process Effects 0.000 description 11
- 238000006731 degradation reaction Methods 0.000 description 11
- 230000003197 catalytic effect Effects 0.000 description 5
- 230000000694 effects Effects 0.000 description 5
- 230000000593 degrading effect Effects 0.000 description 4
- 230000003647 oxidation Effects 0.000 description 4
- 238000007254 oxidation reaction Methods 0.000 description 4
- 239000011941 photocatalyst Substances 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 3
- 238000002474 experimental method Methods 0.000 description 3
- 238000013033 photocatalytic degradation reaction Methods 0.000 description 3
- 230000007281 self degradation Effects 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- 229910021578 Iron(III) chloride Inorganic materials 0.000 description 2
- 238000002441 X-ray diffraction Methods 0.000 description 2
- 239000000969 carrier Substances 0.000 description 2
- 239000003054 catalyst Substances 0.000 description 2
- 229920001940 conductive polymer Polymers 0.000 description 2
- RBTARNINKXHZNM-UHFFFAOYSA-K iron trichloride Chemical group Cl[Fe](Cl)Cl RBTARNINKXHZNM-UHFFFAOYSA-K 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 230000005012 migration Effects 0.000 description 2
- 238000013508 migration Methods 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 239000002957 persistent organic pollutant Substances 0.000 description 2
- 238000005215 recombination Methods 0.000 description 2
- 230000006798 recombination Effects 0.000 description 2
- 238000000926 separation method Methods 0.000 description 2
- 241000282414 Homo sapiens Species 0.000 description 1
- 235000005811 Viola adunca Nutrition 0.000 description 1
- 240000009038 Viola odorata Species 0.000 description 1
- 235000013487 Viola odorata Nutrition 0.000 description 1
- 235000002254 Viola papilionacea Nutrition 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 238000010306 acid treatment Methods 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 238000005256 carbonitriding Methods 0.000 description 1
- 239000011246 composite particle Substances 0.000 description 1
- 239000000356 contaminant Substances 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 230000031700 light absorption Effects 0.000 description 1
- 238000001000 micrograph Methods 0.000 description 1
- 239000004005 microsphere Substances 0.000 description 1
- 238000007146 photocatalysis Methods 0.000 description 1
- 238000013032 photocatalytic reaction Methods 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 239000002861 polymer material Substances 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 238000001228 spectrum Methods 0.000 description 1
- 238000012876 topography Methods 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
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- B01J35/39—
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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
- B01J31/00—Catalysts comprising hydrides, coordination complexes or organic compounds
- B01J31/02—Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides
- B01J31/06—Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides containing polymers
- B01J31/069—Hybrid organic-inorganic polymers, e.g. silica derivatized with organic groups
-
- 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
- B01J31/00—Catalysts comprising hydrides, coordination complexes or organic compounds
- B01J31/26—Catalysts comprising hydrides, coordination complexes or organic compounds containing in addition, inorganic metal compounds not provided for in groups B01J31/02 - B01J31/24
- B01J31/38—Catalysts comprising hydrides, coordination complexes or organic compounds containing in addition, inorganic metal compounds not provided for in groups B01J31/02 - B01J31/24 of titanium, zirconium or hafnium
-
- B01J35/51—
-
- 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
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/40—Organic compounds containing sulfur
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/10—Photocatalysts
Abstract
The invention discloses a polypyrrole/titanium dioxide/graphite phase carbon nitride ternary composite photocatalytic material and a preparation method thereof, and belongs to the technical field of composite materials. The method comprises the following steps: adding carbon nitride powder into concentrated sulfuric acid, and magnetically stirring to prepare an exfoliated graphite-phase carbon nitride nanosheet; centrifugally washing, collecting and drying; preparing the obtained graphite-phase carbon nitride nanosheets into a suspension aqueous solution; in an ice-water bath environment, dispersing titanium dioxide in water, adding pyrrole monomer and adding oxidant; then adding a graphite phase carbon nitride nanosheet suspension aqueous solution, and preparing the polypyrrole/titanium dioxide/graphite phase carbon nitride ternary composite photocatalytic material by using an in-situ polymerization method; after washing, filtering and collecting, and vacuum drying. The invention has the beneficial effects that: simple operation and low cost. The invention of the technology, namely the polypyrrole/titanium dioxide/graphite phase carbon nitride ternary composite photocatalytic material, has wide application prospect in the aspects of sewage treatment and the like as the photocatalytic material.
Description
Technical Field
The invention belongs to the technical field of composite materials, and particularly relates to a method for preparing polypyrrole/titanium dioxide/graphite phase carbon nitride (PPy/TiO)2 / C3N4) A ternary composite photocatalytic material and a preparation method thereof.
Background
The global environmental problem is continuously worsened, the environmental pollution is a global problem which is urgently needed to be solved by human beings in the 21 st century, the photocatalytic reaction can directly use natural resource solar energy as a light source to promote the reaction, and the photocatalytic material is an ideal treatment material due to the unique performance. In order to effectively treat various harmful pollutants in water, the photocatalytic material has always become a research hotspot, has a very wide application prospect, and researchers are dedicated to developing composite photocatalytic materials which have better photocatalytic performance and can be used for multiple times as far as possible.
However, in developing applications, many problems need to be overcome, such as high cost of photodegradable materials and small production volume, and we need to control the cost of raw materials and ensure that the photocatalytic performance is not lost, which needs great improvement
TiO2The photocatalyst which has the advantages of high catalytic efficiency, strong oxidizing property, high cost performance and the like becomes the most widely researched and applied photocatalyst at the present stage, but TiO2Also has limitations, such as pure TiO2The band gap energy is about 3.2eV, and the light energy outside an ultraviolet region cannot be absorbed, so that the utilization of natural sunlight is limited to a great extent; in addition, due to TiO2The presence of strong redox groups, which may result in a high probability of electron-hole pair recombination after the transition, may reduce the catalytic ability.
The graphite phase carbon nitride being C of the graphite phase3N4Composed of C, N elements and having a band gap of about 2.7eV, is often used as a photocatalytic degradation material due to its good stability and easily controlled structure and performance, but graphite-phase carbon nitride as a photocatalyst is not conducive to rapid migration and efficient separation of photo-generated electron-hole pairs, resulting in low photocatalytic efficiency, andthe visible light absorption of graphite phase carbon nitride is mainly concentrated on blue-violet light, and the utilization of visible light is limited, so that the application of graphite phase carbon nitride as a photocatalyst is limited.
Disclosure of Invention
The purpose of the invention is as follows:
in order to solve the technical problem, the polypyrrole/titanium dioxide/graphite phase carbon nitride ternary composite photocatalytic material is obtained based on a conductive polymer material. The titanium dioxide is coated by the polypyrrole, so that the forbidden bandwidth of the titanium dioxide can be reduced, and the polypyrrole/titanium dioxide/graphite phase carbon nitride nanosheet ternary composite material can absorb a wide wavelength range and can reach a visible light region. Meanwhile, the polypyrrole/titanium dioxide/graphite-phase carbon nitride nanosheet ternary composition is more beneficial to enabling photon-generated carriers to migrate from the energy level of a semiconductor, reducing the recombination rate among holes, and enabling electron-hole pairs to be efficiently separated, so that the photocatalytic performance is improved.
The technical scheme is as follows:
the invention discloses a method for preparing polypyrrole/titanium dioxide/graphite phase carbon nitride (PPy/TiO)2 / C3N4) The preparation method of the ternary composite photocatalytic material comprises the following steps:
1) adding carbon nitride into concentrated sulfuric acid, and magnetically stirring for 4-24 hours to prepare the two-dimensional layered graphite phase carbon nitride nanosheet, wherein the sulfuric acid concentration is 98%. Collected after centrifugal washing, 80oAnd C, drying in vacuum to obtain the graphite-phase carbon nitride nanosheet.
2) Placing the device in an ice-water bath, adding a titanium dioxide deionized water suspension solution into a reaction container, and preparing the polypyrrole coated titanium dioxide nano microspheres by using an in-situ chemical oxidation polymerization method, wherein the reaction time is 5min-1h, and the mass ratio of titanium dioxide to pyrrole monomers is 0.05-1.0;
3) in an ice-water bath, adding a graphite phase carbon nitride suspension aqueous solution into the solution in the step 2) by adopting an in-situ chemical oxidation polymerization method, wherein the concentration of the graphite phase carbon nitride suspension aqueous solution is 0.1-100mg/ml, the mass ratio of the graphite phase carbon nitride nanosheets to the pyrrole monomer is 0.05-1.0, the molar ratio of titanium dioxide to the graphite phase carbon nitride is 0.1-10, and the reaction time is 2-8 h.
Preferably, the titanium dioxide is rutile titanium dioxide or anatase titanium dioxide.
Preferably, the oxidant is FeCl3 ●6H2O。
The invention has the beneficial effects that:
the experiment adopts an in-situ oxidation polymerization method and FeCl3.6H2Preparing PPy/TiO with different carbonitriding contents by using O as oxidant2 / C3N4A ternary composite material. By comparing the activity of the sample in photocatalytic degradation of organic pollutant Methylene Blue (MB), the result shows that PPy/TiO is increased along with the increase of polypyrrole content2 / C3N4The light degradation MB effect of the ternary composite material is increased, and the efficiency of degrading methylene blue is more than 99 percent. Due to TiO2With graphite phase C3N4After doping, the doped material is compounded with the conductive polymer PPy, so that the conductivity of the sample is improved, and the migration and separation performance of the photon-generated carriers are improved, thereby improving the degradation efficiency of the sample.
Drawings
FIG. 1 shows the acid-treated graphite-phase carbon nitride (graphite-phase carbon nitride) and carbon nitride (C)3N4) XRD diffractogram of structure;
FIG. 2 shows the production of PPy/TiO2 / C3N4 Scanning electron microscope images of the ternary composite materials;
FIG. 3 is a comparison of the color of a solution of Methylene Blue (MB) for degradation of organic contaminants over different time periods;
FIG. 4 shows PPy/TiO at different times2 / C3N4-3, comparing ultraviolet spectrograms of the ternary composite material degraded methylene blue solution;
FIG. 5 is a plot of the self-degradation of MB without the addition of catalyst material; examples one to three ternary composites and pure TiO2 degradation curves for degrading MB under uv light.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Example one
1) Adding carbon nitride prepared in a laboratory into concentrated sulfuric acid, and magnetically stirring for 4-24 hours to prepare the graphite-phase carbon nitride nanosheet, wherein the concentration of the sulfuric acid is 98%. After centrifugal washing, the mixture is collected and dried in vacuum at 80 ℃ for standby.
2) Placing the device in an ice-water bath, adding 50ml of titanium dioxide deionized water suspension solution into a reaction container of deionized water, wherein the concentration of the titanium dioxide suspension solution is 1mg/ml, sequentially adding 2g of pyrrole monomer, adding FeCl3 ●6H2And O oxidant, and finally adding 50ml of graphite phase carbon nitride suspension aqueous solution with the concentration of 1mg/ml (keeping the molar ratio of the graphite phase carbon nitride to the titanium dioxide to be 1: 1), wherein the reaction time is 5 hours. PPy/TiO preparation by in-situ chemical polymerization2 / C3N4Ternary composite material
Example two
The difference from the first example is that the amount of pyrrole monomer added is 3 ml.
EXAMPLE III
The difference from the first example is that the addition amount of pyrrole monomer is 4ml
Example four
The difference from the first example is that the amount of pyrrole monomer added is 6 ml.
FIG. 1 shows XRD diffraction spectra of graphite phase carbonitride and carbon nitride structures after acid treatment, and 13.1 of XRD spectra of graphite phase carbonitride compared with carbon nitride can be observedoThe peak near the peak disappeared (the stacking peak disappeared), confirming the formation of exfoliated graphite-phase carbon nitride.
FIG. 2 shows that in the third example, the amount of pyrrole added is 4ml, and the molar ratio of graphite phase carbon nitride to oxidation state is kept to 1: 1, PPy/TiO obtained2 / C3N4-3 scanning electron microscope topography of the ternary composite material, canThe composite particles were observed to be uniform in size.
FIG. 3 shows PPy/TiO as a function of time2 / C3N4-3, the color of the catalytic degradation methylene blue solution of the ternary composite material changes, and the color changes to be colorless to indicate that the degradation is finished by the cost.
FIG. 4 PPy/TiO at different times2 / C3N4And (3) comparing ultraviolet spectrograms of the ternary composite material degraded methylene blue solution. The characteristic peak of methylene blue disappeared with increasing time.
FIG. 5PPy/TiO2 / C3N4The activity of the ternary composite material in photocatalytic degradation of organic pollutant Methylene Blue (MB) is tested, as shown in FIG. 3, a MB blank experiment without a catalyst shows that the self-degradation of the methylene blue is about 20% within 1.5h, which indicates that the self-degradation effect is negligible. The degradation experiment is carried out at room temperature in ultraviolet lamp irradiation, the experimental result is shown in figure 3, PPy/TiO increases with the pyrrole content2 / C3N4The effect of the ternary composite material in photocatalysis of methylene blue is improved, wherein PPy/TiO in the third embodiment2 / C3N4The ternary composite material has the best catalytic effect. After 1.5h of degradation, the catalytic effect reaches 99%, and the efficiency of degrading methylene blue by pure titanium dioxide is about 90%. However, when the content of PPy was further increased, the degradation efficiency was slightly decreased as shown in FIG. 5PPy/TiO2 / C3N4-4. All PPy/TiO prepared2 / C3N4The degradation efficiency of the ternary composite material for degrading MB is over 90 percent. Description of PPy/TiO2 / C3N4The degradation efficiency of the ternary composite material is improved.
Claims (8)
1. A preparation method of a polypyrrole/titanium dioxide/graphite phase carbon nitride ternary composite photocatalytic material is characterized by comprising the following steps:
1) adding carbon nitride powder into concentrated sulfuric acid, and magnetically stirring for 4-24 hours to prepare the stripped graphite-phase carbon nitride nanosheet, wherein the concentration of sulfuric acid is 98%;
2) centrifugally washing, collecting and vacuum drying;
3) preparing the graphite-phase carbon nitride nanosheets obtained in the step 2) into a suspension aqueous solution;
4) in an ice-water bath environment, dispersing titanium dioxide in water, adding pyrrole monomer and adding oxidant; then adding a graphite phase carbon nitride nanosheet suspension aqueous solution, reacting for 2-8 h, and preparing the polypyrrole/titanium dioxide/graphite phase carbon nitride ternary composite photocatalytic material by using an in-situ polymerization method;
5) after washing, filtering and collecting, and vacuum drying.
2. The preparation method of the polypyrrole/titanium dioxide/graphite phase carbon nitride three-component composite photocatalytic material according to claim 1, wherein the step 4) comprises the step
4.1) adding deionized water and titanium dioxide into an ice-water bath reactor, and performing ultrasonic dispersion;
4.2) adding pyrrole monomer;
4.3) adding ferric chloride hexahydrate, keeping an ice water bath, and continuously stirring for 5min-1 h;
4.4) adding a graphite phase carbon nitride nanosheet suspension aqueous solution.
3. The preparation method of the polypyrrole/titanium dioxide/graphite phase carbon nitride ternary composite photocatalytic material according to claim 2, wherein the concentration of the graphite phase carbon nitride nanosheet aqueous suspension solution added in the step 4.4) is 0.1-100mg/ml, and the reaction time is 2h-8 h.
4. The preparation method of the polypyrrole/titanium dioxide/graphite phase carbon nitride ternary composite photocatalytic material according to claim 1, wherein the titanium dioxide is rutile titanium dioxide.
5. The method for preparing the polypyrrole/titanium dioxide/graphite phase carbon nitride ternary composite photocatalytic material according to claim 1, wherein the oxidant is ferric chloride hexahydrate.
6. The method for preparing the polypyrrole/titanium dioxide/graphite phase carbon nitride ternary composite photocatalytic material according to claim 2, wherein in the step 4.1), the concentration of the titanium dioxide deionized water solution is 0.1-100 mg/ml.
7. The preparation method of the polypyrrole/titanium dioxide/graphite phase carbon nitride ternary composite photocatalytic material according to claim 1, wherein in the step 4), the mass ratio of titanium dioxide to pyrrole monomer is 0.05-1.0, the molar ratio of titanium dioxide to graphite phase carbon nitride is 0.1-10, and the mass ratio of graphite phase carbon nitride nanosheet to pyrrole monomer is 0.05-1.0.
8. A polypyrrole/titanium dioxide/graphite phase carbon nitride three-component composite photocatalytic material, which is characterized by being prepared by the method of any one of the claims 1 to 7.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN113354868A (en) * | 2021-06-17 | 2021-09-07 | 中山大学 | Phosphorus-doped polypyrrole-loaded carbon nitride nanocomposite and preparation method and application thereof |
| CN113769782A (en) * | 2021-08-16 | 2021-12-10 | 武夷学院 | Preparation method and application of photocatalytic composite material |
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