LU500722B1 - Composite photo Fenton catalyst, preparation method and application thereof - Google Patents
Composite photo Fenton catalyst, preparation method and application thereof Download PDFInfo
- Publication number
- LU500722B1 LU500722B1 LU500722A LU500722A LU500722B1 LU 500722 B1 LU500722 B1 LU 500722B1 LU 500722 A LU500722 A LU 500722A LU 500722 A LU500722 A LU 500722A LU 500722 B1 LU500722 B1 LU 500722B1
- Authority
- LU
- Luxembourg
- Prior art keywords
- composite photo
- fenton catalyst
- deionized water
- photo fenton
- preparation
- Prior art date
Links
Classifications
-
- 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
-
- 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
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/74—Iron group metals
- B01J23/745—Iron
-
- 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
- C02F1/722—Oxidation by peroxides
-
- 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
- C02F1/66—Treatment of water, waste water, or sewage by neutralisation; pH adjustment
-
- 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
- C02F2305/02—Specific form of oxidant
- C02F2305/026—Fenton's reagent
-
- 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
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Hydrology & Water Resources (AREA)
- Life Sciences & Earth Sciences (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Materials Engineering (AREA)
- Health & Medical Sciences (AREA)
- Toxicology (AREA)
- Catalysts (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
Abstract
The invention discloses a composite photo Fenton catalyst, a preparation method and application, which comprises the following steps: preparing Fe3O4; And preparing gC3N4; GC3N4 was dissolved in deionized water, and gC3N4 suspension was obtained by ultrasonic treatment. Dissolving Fe3O4 in deionized water, and performing ultrasonic treatment to obtain Fe3O4 suspension, then dropwise adding Fe3O4 suspension to g-C3N4 suspension, sealing and stirring for 24h to obtain an initial solution, centrifuging and washing the initial solution, and vacuum drying at 60°C for 24h to prepare the composite photo Fenton catalyst; The composite photo Fenton catalyst synthesized by the invention has the characteristics of magnetism, easy separation and recovery, high stability, strong reusability and strong mineralization ability, and the Fe 3 O 4 nanoparticles synthesized by the invention expose more {110} crystal planes, so that the photocatalytic performance is better.
Description
DESCRIPTION Composite photo Fenton catalyst, preparation method and application thereof
TECHNICAL FIELD The invention relates to the technical field of water treatment, in particular to a composite photo Fenton catalyst, a preparation method and an application thereof.
BACKGROUND The widespread existence of antibiotics in water environment poses a potential threat to human health and ecological environment, which makes the removal of trace antibiotics in water become an urgent problem to be solved. In the actual treatment of tetracycline, it is difficult to completely remove tetracycline by traditional techniques such as physical adsorption and biodegradation due to the complexity of post-treatment and 1ts antibacterial property.
Advanced Oxidation (AOPS) technology is regarded as a kind of treatment technology with rich forms, high speed and high efficiency to remove tetracycline from water, including UV/H20,, H202/Fe;+, UV/g-C;N4 and so on. Among them, hydroxyl radicals produced by traditional Fenton reaction can effectively remove tetracycline, but there are some fatal shortcomings, such as iron mud, high iron consumption, low pH , etc. G-C:N4 has a narrow band gap of 2.7eV, which can be used as visible light catalyst. however, due to the high recombination rate of photogenerated electrons and holes, its photocatalytic performance is affected.
In view of the above defects, the author of the present invention finally obtained the present invention after a long period of research and practice.
SUMMARY To solve the above technical defects, the technical scheme adopted by the present invention is to provide a preparation method of the composite photo Fenton catalyst, which comprises the following steps: S1, dissolving FeSO4:7H:0 and Na2S203-5H;0 in deionized water to obtain a first aqueous solution, and dissolving NaOH in deionized water; obtaining a second aqueous solution in ionic water, mixing and stirring the first aqueous solution and the second aqueous solution to obtain a reaction solution, transferring the reaction solution to an autoclave, sealing and keeping for 12 h at 140°C, then cooling to room temperature, finally washing with deionized water for 3-4 times, and drying in a vacuum oven at 60°C for 4 h to prepare Fes Oy; S2, placing urea in a crucible, heating to 550°C at a heating rate of 5°C/min in a muffle furnace, keeping the temperature constant for 2h, cooling to room temperature, and grinding to obtain g-C3N4; S3, dissolving g-C3;N4 in deionized water, and performing ultrasonic treatment to obtain g-C3N4 suspension; dissolving Fe304 in deionized water, performing ultrasonic treatment to obtain Fe304 suspension, dropwise adding the Fe:04 suspension to the g- C3N4 suspension, sealing and stirring for 24h to obtain an initial solution, centrifuging and washing the initial solution, and vacuum drying at 60°C for 24h to prepare the composite photo Fenton catalyst.
Preferably, in the preparation process of the first aqueous solution, FeSO4-7H20 is 1. 20g-3. 50g, Na2S203-.
SH20 is 1. 10g-2.50g, and deionized water is 15mL-30mL.
Preferably, in the preparation process of the second aqueous solution, NaOH is 0 .2g-0 49, and deionized water is 10mL- 30mL.
Preferably, in S1, the mixing and stirring time of the first aqueous solution and the second aqueous solution is 3 min to 7 min.
Preferably, in S3, 90 mg-99 mg of g-C3N4 1s dissolved in SOmL of deionized water, and 1mg- 10mg of Fe30y4 is dissolved in 10mL of deionized water.
Preferably, the composite photo Fenton catalyst is prepared by the preparation method of the composite photo Fenton catalyst, and the composite photo Fenton catalyst is Fe304/g-C3N4.
Preferably, the composite photo Fenton catalyst is used for removing tetracycline in water.
Compared with the prior art, the invention has the beneficial effects that under the visible light condition, Fe3O4/g-C3N4 catalyzes hydrogen peroxide to generate hydroxyl radicals and superoxide radicals to degrade tetracycline hydrochloride. The composite photo Fenton catalyst synthesized by the invention has the characteristics of magnetism,
easy separation and recovery, high stability, strong reusability and strong mineralization ability, and the Fe304 nanoparticles synthesized by the invention expose more {110} crystal planes, so that the photocatalytic performance is better. Within 100min, Fe304/g- C3N4 can degrade the total organic carbon of tetracycline hydrochloride by 67. 1%, which can transform tetracycline hydrochloride into harmless small molecules. In addition, after five repeated experiments, the removal rate can reach 87. 9%, which shows that Fe304/g- C3N4 has excellent activity, and the iron leaching rate is very low and the stability is good. According to the invention, Fe304/g-C;N4 is used as a photoFenton reagent for treating tetracycline antibiotics in water, and has a good application prospect.
BRIEF DESCRIPTION OF THE FIGURES Fig. 1 is a scanning electron microscope of Fe304/g-C3N4; Fig. 2 is an electron microscope scan of Fe304 generated in S1; Fig. 3 is a comparison diagram of degradation rates of tetracycline hydrochloride by Fe;O4/g-C3N4 generated by the present invention and common Fe304/g-C3N4 under visible light; Fig. 4 is a comparative diagram of the effects of FezO4/g-C;N4 pHoto Fenton material generated by the present invention on the degradation of tetracycline hydrochloride under different pH conditions; Fig. 5 is a comparative diagram of the effects of Fez04/g-C:N4 photo Fenton material generated by the present invention on the degradation of tetracycline hydrochloride under different HO, dosage; Fig. 6 is a comparative diagram of the removal rates of tetracycline hydrochloride and total organic carbon by Fe304/g-C3N4 produced by the present invention after five times of reuse; Fig. 7 is a comparative diagram of Fes04/g-C3N4 reaction degradation under sunlight and visible light.
DESCRIPTION OF THE INVENTION The above and other technical features and advantages of the present invention will be described in more detail with reference to the accompanying drawings.
Example 1
The composite photo Fenton catalyst is a Fe304/g-C;N4 photo Fenton material, and the preparation method of the Fe304/g-C;N4 photo Fenton material specifically comprises the following steps: S1, dissolving 1 .39g of FeSO4 7H20 and 1 .24g of Na2S203-S5H,0 in 15mL of deionized water and O0 .4g of NaOH. After mixing and stirring in 10mL deionized water for about Smin, the reacted solution was transferred to a 50ml autoclave, sealed at 140°C and kept for 12h, and then cooled to room temperature. Finally, Fes04 was prepared by washing with deionized water for 3-4 times and drying in a vacuum oven at 60°C for 4 hours.
S2, placing 15g of urea in a crucible, heating to 550°C at a heating rate of 5°C/min in a muffle furnace, keeping the temperature constant for 2h, cooling to room temperature, and grinding to obtain g-C3N4.
S3, dissolving 93mg of g-C3Ny in 50mL of deionized water, and performing ultrasonic treatment for 30min; dissolving 7mg of FesO4 in 10mL deionized water, and carry out ultrasonic treatment for 15min. Then, Fe304 suspension was added dropwise to g-C3N4 suspension, and the mixture was stirred hermetically for 24h. The product was centrifuged, washed and dried in vacuum at 60°C for 24h to obtain Fe304/g-C3N4.
As shown in fig. 1, fig. 1 is a scanning electron micrograph of FesO4/g-C3Ny. the Fe3O4/g-C3N4 prepared by the present invention is powder with larger specific surface area and more active sites.
As shown in fig. 2, fig. 2 is an electron microscope scan of FesO4 generated in S1. It can be seen that FesO4 produced by the invention is polyhedral and has 11 {110} crystal planes, 8 {111} crystal planes and 6 {100} crystal planes. Generally speaking, the final size and shape of micro-nanocrystals are the result of competition between nucleation and growth in the crystal growth stage, which are determined by the intrinsic crystal structure of the products and the chemical potential of the reaction process. The key factor to control the morphology of nanoparticles is to control the growth direction of crystal plane. From the crystallographic point of view, FesO4 belongs to face-centered cubic structure, which obeys the following crystal plane energy rule: y{111} <y{100} <y{110}. It also shows that the {111} crystal plane is in the lowest energy state, the {110} crystal plane is in the highest energy state, and the {100} crystal plane is in between. Therefore, compared with ordinary spherical Fe304 particles, Fe304 generated by the invention exposes more high-energy {110} crystal planes and has better photocatalytic performance.
As shown in fig. 3, fig. 3 is a comparison chart of degradation rates of tetracycline hydrochloride by Fe304/g-C3N4 produced by the present invention and ordinary FesOwg- C3N4 under visible light. As shown in the figure, Fe304 in the {110}-Fe304/g-C3N4 produced by the present invention exposes a high-energy {110} crystal plane, and has better photocatalytic performance. Compared with Fe304/g-C3N4 synthesized by ordinary FezO4, the degradation rate of tetracycline hydrochloride is increased by 40. 2% within 100 minutes.
Example 2 Experimental process of degradation of tetracycline hydrochloride in water by Fez04/g-C3N4 photo Fenton material; Al, firstly adjust the pH of tetracycline hydrochloride solution, then add a certain amount of Fe304/g-C3Ny into 50mL tetracycline hydrochloride solution, and stir in the dark for 30min.
A2, add a certain amount of H20,, turn on the lamp to react for 100min, and collect ImL of reaction suspension samples every 20min. The obtained samples were filtered and the concentration of tetracycline hydrochloride was determined.
When tetracycline hydrochloride was removed, the dosage of Fe304/g-C3N4 ranged from 0.5g/1 to 2.0g/1.
When removing tetracycline hydrochloride, the initial concentration of tetracycline hydrochloride in the system was 25 mg/l-85 mg/l.
As shown in fig. 4, fig. 4 is a comparative diagram of the effects of Fe:04/g-C3N4 Photo Fenton material generated by the present invention on the degradation of tetracycline hydrochloride under different pH conditions; under the condition of pH = 2- 5, the removal rate of tetracycline hydrochloride by the composite photo Fenton catalyst of the invention is over 90%. The removal rate can reach 70%-80% even when the pH value is close to neutral. It can be known from fig. 4 that the pH of the composite pHoto Fenton catalyst of the present invention is not high, which enlarges the application range of the photo Fenton catalyst, realizes the reaction without adjusting the pH, and reduces the operation cost.
As shown in fig. 5, fig. 5 is a comparative diagram of the effects of Fe:04/g-C3N4 photo Fenton material generated by the present invention on the degradation of tetracycline hydrochloride under different H202 dosage. As shown in the figure, under the condition of HO, = 5 mmol/L, the removal rate of tetracycline hydrochloride by the composite photo Fenton catalyst of the present invention reaches 98%. Under the condition of HO, = 3mmol/l, the removal rate can reach 95%. However, the traditional homogeneous Fenton reaction generally requires the concentration of H:O, to be 10 mmol/L-20 mmol/L, and the concentration of H20> only needs 3 mmol/L-5 mmol/L when using this catalyst, which reduces the operation cost.
As shown in fig. 6, fig. 6 is a comparative diagram of the removal rates of tetracycline hydrochloride and total organic carbon by Fe304/g-C;N4 generated by the present invention after five times of reuse. After being reused for five times, Fe:O4/g- C3N4 still has strong activity on degradation and mineralization of tetracycline hydrochloride. After six uses, the degradation efficiency of tetracycline hydrochloride ranged from 98. 8% to 87. 9%, and the salinity of tetracycline hydrochloride ranged from
67. 1% to 57. 1%. This shows that Fe3z04/g-C3N4 as photoFenton reagent has good stability and reusability in degrading tetracycline hydrochloride.
As shown in fig. 7, fig. 7 is a comparison diagram of Fez04/g-C3N4 generated by the present invention under sunlight and visible light. The degradation efficiency of tetracycline hydrochloride is 99. 7% under sunlight for 60min, which is faster than that under visible light, which indicates that Fes04/g-C3N4 as photoFenton reagent has a better practical application prospect.
The above is only a preferred embodiment of the present invention, which is only illustrative and not restrictive to the present invention. The skilled person understands that many changes, modifications and even equivalents can be made within the spirit and scope defined by the claims of the present invention, but they will all fall within the protection scope of the present invention.
Claims (7)
1. A preparation method of a composite photo Fenton catalyst, which is characterized by comprising the following steps: sl, dissolving FeSO4-7H>0 and Na»>S:03-5H»0 in deionized water to obtain a first aqueous solution, dissolving NaOH in deionized water to obtain a second aqueous solution, mixing and stirring the first aqueous solution and the second aqueous solution to obtain a reaction solution, transferring the reaction solution to an autoclave, sealing and maintaining for 12 h at 140°C, then cooling to room temperature, finally washing with deionized water, and drying in a vacuum oven at 60°C for 4h to obtain Fez3O4; s2, placing urea in a crucible, heating to 550°C at a heating rate of 5°C/min in a muffle furnace, keeping the temperature constant for 2h, cooling to room temperature, and grinding to obtain g-C3N4; s3, dissolving g-C3N4 in deionized water, and performing ultrasonic treatment to obtain g-C3N4 suspension; dissolving Fe304 in deionized water, performing ultrasonic treatment to obtain Fe304 suspension, dropwise adding the Fe304 suspension to the g- C3N4 suspension, sealing and stirring for 24h to obtain an initial solution, centrifuging and washing the initial solution, and vacuum drying at 60°C for 24h to prepare the composite photo Fenton catalyst.
2. The preparation method of the composite photo Fenton catalyst according to claim 1, wherein in the preparation process of the first aqueous solution, FeSO4:7H20 is
1. 20g-3.50g, Na2S203 -5H20 1s 1. 10g-2.50g, and deionized water is 15mL-30mL.
3. The preparation method of the composite photo Fenton catalyst according to claim 1, wherein in the preparation process of the second aqueous solution, NaOH is 0.2 g-0.4 g, and deionized water is 10 mL-30 mL.
4. The preparation method of the composite photo Fenton catalyst according to claim 1, wherein in sl, the mixing and stirring time of the first aqueous solution and the second aqueous solution is 3 min- 7 min.
5. The preparation method of the composite photo Fenton catalyst according to claim 1, wherein in s3, 90 mg-99 mg of g-C3N4 is dissolved in 50 mL of deionized water, and 1 mg-10mg of Fe30y4 is dissolved in 10mL of deionized water.
6. A composite photo Fenton catalyst, which is prepared by the preparation method of the composite photo Fenton catalyst according to any one of claims 1-5, wherein the composite photo Fenton catalyst is Fe304/g-C3N4.
7. The application of the composite photo Fenton catalyst according to any one of claims 1-6, which is used for removing tetracycline in water.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| LU500722A LU500722B1 (en) | 2021-10-12 | 2021-10-12 | Composite photo Fenton catalyst, preparation method and application thereof |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| LU500722A LU500722B1 (en) | 2021-10-12 | 2021-10-12 | Composite photo Fenton catalyst, preparation method and application thereof |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| LU500722B1 true LU500722B1 (en) | 2022-04-12 |
Family
ID=81127811
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| LU500722A LU500722B1 (en) | 2021-10-12 | 2021-10-12 | Composite photo Fenton catalyst, preparation method and application thereof |
Country Status (1)
| Country | Link |
|---|---|
| LU (1) | LU500722B1 (en) |
-
2021
- 2021-10-12 LU LU500722A patent/LU500722B1/en active IP Right Grant
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| CN108311153B (en) | Nano-ZnO loaded magnetic biochar composite photocatalyst and preparation method thereof | |
| CN111495367B (en) | Magnetic polyaniline-porous carbon-Fe 3 O 4 Preparation method and application of photo-Fenton catalyst | |
| CN107758836B (en) | Method for removing refractory organic matters through in-situ coupling of microbial fuel cell and persulfate Fenton technology | |
| CN110787645B (en) | Visible light photocatalyst modified PVDF ultrafiltration membrane as well as preparation method and application thereof | |
| CN111760569A (en) | Composite photo-Fenton catalyst, preparation method and application | |
| CN109999752B (en) | Preparation method and application of multifunctional material for efficiently adsorbing and degrading organic pollutants | |
| CN108452820B (en) | Carbon nitride/alpha-type iron oxide catalyst, photoelectric auxiliary Fenton-like system and application of photoelectric auxiliary Fenton-like system in organic wastewater treatment | |
| CN112056310B (en) | DFNS (double-walled carbon nanotubes) loaded carbon quantum dot/molybdenum disulfide quantum dot as well as preparation method and application thereof | |
| CN114225938A (en) | Magnetic nano Fe3O4@ mushroom residue biochar Fenton catalyst and preparation method thereof | |
| CN110756163A (en) | Nano CoFe2O4Carbon fiber felt composite material and preparation method and application thereof | |
| CN110064407A (en) | Biological preparation method based on zinc-manganese ferrite loaded nano copper sulfide | |
| CN110075929B (en) | Preparation method of polyacid intercalation 3D-LDHs photo-Fenton catalyst | |
| CN111439807A (en) | Visible light catalysis water body disinfection method based on multi-element composite material | |
| CN112156764A (en) | Nano TiO (titanium dioxide)2Modified graphene oxide/organic bentonite composite material and preparation method thereof | |
| LU500722B1 (en) | Composite photo Fenton catalyst, preparation method and application thereof | |
| CN108940348B (en) | Silver chromate/sulfur-doped nitrogen carbon Z-type photocatalyst and preparation method thereof | |
| CN117718018A (en) | Composite aerogel for adsorbing Cu in water and preparation method thereof | |
| CN115814829B (en) | Co and Mo2C-codoped biochar-based composite material and preparation method and application thereof | |
| CN108383208B (en) | Method for treating organic wastewater by virtue of micro-battery-Fenton-like system | |
| CN114177911B (en) | Carbon-supported multi-metal oxide catalyst and preparation method and application thereof | |
| CN114377696B (en) | Biofilm-based BiOCl x Br (1-x) /Au/MnO 2 Composite material, preparation method and application thereof | |
| CN106587325B (en) | By using CoxFe1-xMethod for treating refractory wastewater by using P material heterogeneous activated monopersulfate | |
| CN115121239A (en) | Preparation method and application of biochar catalyst | |
| CN114797862A (en) | Iron-based pig blood carbon quantum dot composite transition metal catalyst and preparation method and application thereof | |
| CN115245839A (en) | Preparation method of phosphomolybdic acid intercalated 3D-LDHs photo-Fenton catalyst |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| FG | Patent granted |
Effective date: 20220412 |