CN112058295A - Diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous catalyst, application thereof and in-situ preparation method - Google Patents
Diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous catalyst, application thereof and in-situ preparation method Download PDFInfo
- Publication number
- CN112058295A CN112058295A CN202010817724.0A CN202010817724A CN112058295A CN 112058295 A CN112058295 A CN 112058295A CN 202010817724 A CN202010817724 A CN 202010817724A CN 112058295 A CN112058295 A CN 112058295A
- Authority
- CN
- China
- Prior art keywords
- diaminopyridine
- oxide
- ferroferric oxide
- sinter
- praseodymium
- 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.)
- Granted
Links
Images
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
-
- 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
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/02—Impregnation, coating or precipitation
- B01J37/0201—Impregnation
- B01J37/0203—Impregnation the impregnation liquid containing organic 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
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/08—Heat treatment
- B01J37/082—Decomposition and pyrolysis
-
- 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
- C02F1/72—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
-
- 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
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Materials Engineering (AREA)
- Life Sciences & Earth Sciences (AREA)
- Hydrology & Water Resources (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Physics & Mathematics (AREA)
- Thermal Sciences (AREA)
- Catalysts (AREA)
Abstract
The invention discloses a diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous catalyst, and application and an in-situ preparation method thereof. Different techniques of biological treatment, fenton method, adsorption, etc. have been studied to remove ibuprofen, but these methods require a large amount of energy and generate secondary pollution. The invention provides a novel catalyst for loading praseodymium oxide and diaminopyridine sinter on ferroferric oxide, which can activate peroxydisulfate to generate free radicals to degrade ibuprofen by a catalytic synergistic effect, and the catalytic efficiency is obviously higher than that of the existing ferroferric oxide catalyst. In addition, the method has the advantages of short treatment time, high degradation efficiency, no secondary pollution generation, no need of pH value adjustment and good practical application prospect. According to the invention, the diaminopyridine sinter compound praseodymium oxide and ferroferric oxide heterogeneous Fenton catalyst is synthesized by an in-situ impregnation method, the required equipment condition is low, and the preparation process is simple and convenient.
Description
Technical Field
The invention belongs to the technical field of pharmaceutical wastewater treatment, and particularly relates to an in-situ preparation of a high-efficiency 2, 6-diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous Fenton catalyst.
Background
Recently, trace amounts of pharmaceutical and personal care products such as anti-inflammatory drugs, analgesics, and antibiotics have been found in water supplies. The concentration of these contaminants is as high as 10. mu.g.L-1Their existence has attracted a great deal of attention. Among these organic pollutants, ibuprofen is one of the most widely consumed drugs worldwide and is used for alleviating symptoms such as arthritis, primary dysmenorrhea, fever and analgesia, especially for curing inflammatory diseases.
Due to the toxic effect of ibuprofen, the most important requirement is to remove the ibuprofen drug residue from the waste water. Various techniques of biological treatment, fenton method, adsorption, etc. have been studied to remove ibuprofen, but these methods require a large amount of energy and generate secondary pollution. Recently, advanced oxidation processes have become a promising alternative to conventional technologies due to their superior processing efficiency. Advanced oxidation technologies mainly utilize active radicals with extremely strong oxidizing power to oxidize and decompose pollutants difficult to degrade in water, wherein the advanced oxidation technologies based on sulfate radicals are strongly concerned due to the fact that the generated sulfate radicals have longer service life and stronger oxidizing power.
The iron oxide catalyst can be used as a heterogeneous catalyst to activate peroxydisulfate to generate free radicals and remove a series of organic pollutants. Compared with other iron oxides, the ferroferric oxide has the unique properties of stable physical and chemical structure, lower preparation cost, easy synthetic process, magnetic response and the like. However, the pure ferroferric oxide catalyst has the defects of slow degradation kinetics, and limited agglomeration and active site exposure. In order to solve the problems that ibuprofen is poor in removal effect and a Fenton-like catalyst is difficult to separate and recycle in conventional sewage treatment, the technology of generating 2, 6-diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous Fenton-like catalyst in situ is utilized, ferroferric oxide, praseodymium oxide and carbon nitrogen sintering materials are combined, and the synergistic effect of the materials is utilized to accelerate the reaction, so that organic pollutants which are difficult to biodegrade in water are removed durably and efficiently.
Disclosure of Invention
The invention aims to provide a method for preparing a high-efficiency carbon-nitrogen co-doped ferroferric oxide heterogeneous Fenton catalyst in situ and application thereof.
The invention relates to a diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous catalyst, which comprises ferroferric oxide and praseodymium oxide and diaminopyridine sinter loaded on the ferroferric oxide.
Preferably, the sintered praseodymium oxide and diaminopyridine are obtained by loading praseodymium salt and diaminopyridine on ferroferric oxide and then calcining the mixture.
Preferably, the temperature of calcination is 500 ℃.
Preferably, the mass fraction of the ferroferric oxide is 62.5%, the mass fraction of the praseodymium oxide is 31.25%, and the mass fraction of the diaminopyridine sinter is 6.25%.
The application of the diaminopyridine sinter compound praseodymium oxide and ferroferric oxide heterogeneous catalyst in degradation of ibuprofen is as follows:
step one, adding an oxidant into the ibuprofen wastewater.
And step two, adding the diaminopyridine sinter compound praseodymium oxide and ferroferric oxide heterogeneous catalyst into the carbamazepine wastewater to decompose the ibuprofen.
Preferably, the ibuprofen waste water is continuously stirred in steps one and two. The oxidant in the first step is sodium persulfate. In the second step, the carbamazepine wastewater is kept at 20-30 ℃ for reaction.
The in-situ preparation method of the diaminopyridine sinter compound praseodymium oxide and ferroferric oxide heterogeneous catalyst in degradation of ibuprofen comprises the following steps:
step one, adding ferroferric oxide powder into a praseodymium nitrate and diaminopyridine mixed solution, and soaking until drying to obtain precursor powder.
Step two, calcining the precursor powder; calcining and cooling to obtain the diaminopyridine sinter compound praseodymium oxide and ferroferric oxide heterogeneous catalyst.
Preferably, the first step is carried out by immersing in a water bath at 80 ℃.
Preferably, the temperature rise rate of the calcination is 3 ℃ per minute, and the calcination temperature is 300-700 ℃; the calcination time was 3 hours.
Preferably, the preparation process of the ferroferric oxide powder in the first step is as follows: FeSO (ferric oxide) is added4·7H2O and FeCl3·6H2Preheating the mixed solution of O to a preset temperature, and dropwise adding the mixed solution of O into an ammonia water solution subjected to water bath ultrasonic treatment at the preset temperature. After the titration is finished, the mixture is continuously subjected to water bath ultrasonic treatment at the preset temperature. And then naturally cooling the mixture to room temperature, centrifugally washing, drying the obtained catalyst, and grinding to obtain ferroferric oxide powder.
The invention has the beneficial effects that:
1. the invention provides a novel catalyst for loading praseodymium oxide and diaminopyridine sinter on ferroferric oxide, which can activate peroxydisulfate to generate free radicals to degrade ibuprofen by a catalytic synergistic effect, and the catalytic efficiency is obviously higher than that of the existing ferroferric oxide catalyst. In addition, the novel catalyst provided by the invention is used for carrying out catalytic degradation on the pharmaceutical compound by a Fenton-like method, has short treatment time and high degradation efficiency, does not generate secondary pollution, does not need to adjust the pH value, and has better practical application prospect.
2. According to the invention, the diaminopyridine sinter compound praseodymium oxide and ferroferric oxide heterogeneous Fenton catalyst is synthesized by an in-situ impregnation method, the required equipment condition is low, and the preparation process is simple and convenient.
3. The invention evaluates the influence of the calcination temperature on the activity of the diaminopyridine sinter praseodymium oxide and ferroferric oxide heterogeneous Fenton catalyst, provides 500 ℃ as the optimal sintering temperature, and the catalytic efficiency of the obtained catalyst is obviously higher than that of the catalyst obtained at other sintering temperatures.
Drawings
Figure 1 is the degradation efficiency of different catalysts for ibuprofen.
Detailed Description
The invention is further described below with reference to the accompanying drawings.
Example 1
The preparation method of the in-situ prepared efficient 2, 6-diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous Fenton catalyst comprises the following steps:
(1) solution preparation:
a. respectively configure 1mol and L-1FeCl3·6H2O solution and 1 mol. L-1FeSO4·7H2O solution 10mL each.
b. Preparation of 3 mol. L-145mL of ammonia solution.
c. The solution was disposed at 0.83 mmol. multidot.L-12, 6-diaminopyridine with 2 mol. L-1Pr (NO)3)3·6H20.5mL of the mixed solution of O.
(2) Preparing ferroferric oxide powder: the FeSO with quantitative proportion is added4·7H2O and FeCl3·6H2Preheating the mixed solution of O to 60 ℃, and dropwise adding the mixed solution of O into an ammonia water solution subjected to water bath ultrasonic treatment at 60 ℃. After the titration, the mixture was subjected to ultrasonic treatment in a water bath at 60 ℃ for 30 min. And then naturally cooling the mixture to room temperature, centrifugally washing, putting the obtained catalyst into a vacuum oven for drying for 12 hours, finally taking out the catalyst, grinding the catalyst, and storing the catalyst under a nitrogen sealing condition to obtain ferroferric oxide powder.
(3) Preparation of an impregnation precursor: and adding 0.1g of ferroferric oxide powder into 0.5mL of a mixed solution of praseodymium nitrate and 2, 6-diaminopyridine, and soaking in a water bath at 80 ℃ until the powder is completely dried to obtain precursor powder.
(4) And (3) calcining: and calcining the dried precursor powder in a tubular furnace at the temperature rising rate of 3 ℃ per minute from the ambient temperature to 500 ℃, keeping the temperature for 3 hours, cooling to room temperature, taking out the powder catalyst, and grinding to obtain the 2, 6-diaminopyridine sinter compound praseodymium oxide and ferroferric oxide catalyst. In the obtained 2, 6-diaminopyridine sinter composite praseodymium oxide and ferroferric oxide catalyst, the mass fraction of ferroferric oxide is 62.5 percent, the mass fraction of praseodymium oxide is 31.25 percent, and the mass fraction of diaminopyridine sinter is 6.25 percent
The process for degrading ibuprofen by a fenton-like (sodium persulfate) method for the 2, 6-diaminopyridine sinter composite praseodymium oxide and ferroferric oxide catalyst prepared in the embodiment is as follows:
dissolving ibuprofen in water, ultrasonically stirring for dissolving to obtain solution with concentration of 10 mg.L-1Adding 100mL of ibuprofen solution into a 250mL conical flask, simultaneously adding 25mg of sodium persulfate, and uniformly stirring and dissolving. 20mg of the high-efficiency 2, 6-diaminopyridine sinter compound praseodymium oxide and ferroferric oxide heterogeneous Fenton catalyst prepared in the embodiment is added into a conical flask, the conical flask is placed in a temperature-controlled shaking table to react for 60min (25 ℃, 250r/min), and sampling analysis is carried out every 5min in the reaction process, and the result is shown in figure 1.
Example 2
The preparation method of the in-situ prepared efficient 2, 6-diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous Fenton catalyst comprises the following steps:
(1) solution preparation:
a. respectively configure 1mol and L-1FeCl3·6H2O solution and 1 mol. L-1FeSO4·7H2O solution 10mL each.
b. Preparation of 3 mol. L-145mL of ammonia solution.
c. The solution was disposed at 0.83 mmol. multidot.L-12, 6-diaminopyridine with 2 mol. L-1Pr (NO)3)3·6H20.5mL of the mixed solution of O.
(2) Preparing ferroferric oxide powder: the FeSO with quantitative proportion is added4·7H2O and FeCl3·6H2Preheating the mixed solution of O to 60 ℃, and dropwise adding the mixed solution into a water bath at 60 DEG CAnd (4) ultrasonic treatment of the ammonia water solution to obtain a mixture. After the titration, the mixture was subjected to ultrasonic treatment in a water bath at 60 ℃ for 30 min. And then naturally cooling the mixture to room temperature, centrifugally washing, putting the obtained catalyst into a vacuum oven for drying for 12 hours, finally taking out the catalyst, grinding the catalyst, and storing the catalyst under a nitrogen sealing condition to obtain ferroferric oxide powder.
(3) Preparation of an impregnation precursor: and adding 0.1g of ferroferric oxide powder into 0.5mL of a mixed solution of praseodymium nitrate and 2, 6-diaminopyridine, and soaking in a water bath at 80 ℃ until the powder is completely dried to obtain precursor powder.
(4) And (3) calcining: and calcining the dried precursor powder in a tubular furnace at the temperature rising rate of 3 ℃ per minute from the ambient temperature to 300 ℃, keeping the temperature for 3 hours, cooling to room temperature, taking out the powder catalyst, and grinding to obtain the 2, 6-diaminopyridine sinter compound praseodymium oxide and ferroferric oxide catalyst.
The process for degrading ibuprofen by a fenton-like (sodium persulfate) method for the 2, 6-diaminopyridine sinter composite praseodymium oxide and ferroferric oxide catalyst prepared in the embodiment is as follows:
dissolving ibuprofen in water, ultrasonically stirring for dissolving to obtain solution with concentration of 10 mg.L-1Adding 100mL of ibuprofen solution into a 250mL conical flask, simultaneously adding 25mg of sodium persulfate, and uniformly stirring and dissolving. 20mg of the high-efficiency 2, 6-diaminopyridine sinter compound praseodymium oxide and ferroferric oxide heterogeneous Fenton catalyst prepared in the embodiment is added into a conical flask, the conical flask is placed in a temperature-controlled shaking table to react for 60min (25 ℃, 250r/min), and sampling analysis is carried out every 5min in the reaction process, and the result is shown in figure 1.
Example 3
The preparation method of the in-situ prepared efficient 2, 6-diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous Fenton catalyst comprises the following steps:
(1) solution preparation:
a. respectively configure 1mol and L-1FeCl3·6H2O solution and 1 mol. L-1FeSO4·7H2O solution10mL each.
b. Preparation of 3 mol. L-145mL of ammonia solution.
c. The solution was disposed at 0.83 mmol. multidot.L-12, 6-diaminopyridine with 2 mol. L-1Pr (NO)3)3·6H20.5mL of the mixed solution of O.
(2) Preparing ferroferric oxide powder: the FeSO with quantitative proportion is added4·7H2O and FeCl3·6H2Preheating the mixed solution of O to 60 ℃, and dropwise adding the mixed solution of O into an ammonia water solution subjected to water bath ultrasonic treatment at 60 ℃ to obtain a mixture. After the titration, the mixture was subjected to ultrasonic treatment in a water bath at 60 ℃ for 30 min. And then naturally cooling the mixture to room temperature, centrifugally washing, putting the obtained catalyst into a vacuum oven for drying for 12 hours, finally taking out the catalyst, grinding the catalyst, and storing the catalyst under a nitrogen sealing condition to obtain ferroferric oxide powder.
(3) Preparation of an impregnation precursor: and adding 0.1g of ferroferric oxide powder into 0.5mL of a mixed solution of praseodymium nitrate and 2, 6-diaminopyridine, and soaking in a water bath at 80 ℃ until the powder is completely dried to obtain precursor powder.
(4) And (3) calcining: and calcining the dried precursor powder in a tubular furnace at the temperature rising rate of 3 ℃ per minute from the ambient temperature to 700 ℃, keeping the temperature for 3 hours, cooling to room temperature, taking out the powder catalyst, and grinding to obtain the 2, 6-diaminopyridine sinter compound praseodymium oxide and ferroferric oxide catalyst.
The process for degrading ibuprofen by a fenton-like (sodium persulfate) method for the 2, 6-diaminopyridine sinter composite praseodymium oxide and ferroferric oxide catalyst prepared in the embodiment is as follows:
dissolving ibuprofen in water, ultrasonically stirring for dissolving to obtain solution with concentration of 10 mg.L-1Adding 100mL of ibuprofen solution into a 250mL conical flask, simultaneously adding 25mg of sodium persulfate, and uniformly stirring and dissolving. The high-efficiency 2, 6-diaminopyridine sinter compound praseodymium oxide and ferroferric oxide heterogeneous Fenton catalyst prepared in example 4 is added into a conical flask and placed in a temperature-controlled shaking table to react for 60min (25 ℃, 250r/min), and the reaction is carried out every 5min in the reaction processThe line sampling analysis results are shown in FIG. 1.
Comparative example
The preparation method of the pure ferroferric oxide catalyst comprises the following steps:
(1) solution preparation:
a. respectively configure 1mol and L-1FeCl3·6H2O solution and 1 mol. L-1FeSO4·7H2O solution 10mL each.
b. Preparation of 3 mol. L-145mL of ammonia solution.
(2) Preparing ferroferric oxide powder: the FeSO with quantitative proportion is added4·7H2O and FeCl3·6H2The mixed solution of O (molar amount 1:1 ratio in this example) was preheated to 60 ℃ and added dropwise to an aqueous ammonia solution subjected to ultrasonic treatment in a water bath at 60 ℃ to form a mixture. After the titration, the mixture was subjected to ultrasonic treatment in a water bath at 60 ℃ for 30 min. And then naturally cooling the mixture to room temperature, centrifugally washing, putting the obtained catalyst into a vacuum oven for drying for 12 hours, finally taking out the catalyst, grinding the catalyst, and storing the catalyst under a nitrogen sealing condition to obtain the pure ferroferric oxide catalyst.
The pure ferroferric oxide catalyst prepared in the example 1 is used for degrading ibuprofen by a fenton-like (sodium persulfate) method, and the process is as follows:
dissolving ibuprofen in water, ultrasonically stirring for dissolving to obtain solution with concentration of 10 mg.L-1Adding 100mL of ibuprofen solution into a 250mL conical flask, simultaneously adding 25mg of sodium persulfate, and uniformly stirring and dissolving. 20mg of the ferroferric oxide catalyst prepared in example 1 is added into a conical flask, the conical flask is placed in a temperature-controlled shaking table to react for 60min (25 ℃, 250r/min), and sampling analysis is carried out every 5min in the reaction process.
The invention utilizes the in-situ prepared high-efficiency 2, 6-diaminopyridine sinter compound praseodymium oxide and ferroferric oxide catalysis synergistic effect to activate the peroxydisulfate to generate free radicals to degrade ibuprofen. The advantages of the catalyst prepared by the invention on the catalytic degradation effect of ibuprofen are demonstrated by combining specific experiments.
The 2, 6-diaminopyridine sinter composite praseodymium oxide and ferroferric oxide catalyst prepared in examples 1 to 3, the pure ferroferric oxide catalyst prepared in the comparative example, only sodium Persulfate (PS) without adding the catalyst, and the degradation effect on ibuprofen compared with the case are shown in fig. 1. As can be seen from fig. 1, ibuprofen is substantially not degraded by PS without the addition of a catalyst. Under the catalytic action of a pure ferroferric oxide catalyst, ibuprofen is partially degraded, but the residual ibuprofen is higher than 50% after 30 minutes.
The 2, 6-diaminopyridine sinter composite praseodymium oxide and ferroferric oxide catalyst prepared in the embodiment 1-3 have better catalytic degradation effect on ibuprofen than a pure ferroferric oxide catalyst; this indicates that the synergistic effect of the ferroferric oxide, praseodymium oxide and the carbon-nitrogen sintered material is beneficial to activating the peroxydisulfate to generate free radicals to degrade pollutants.
In particular, the '2, 6-diaminopyridine sinter praseodymium oxide and ferroferric oxide catalyst' (sintering temperature of 500 ℃) prepared in example 2 has the advantage that the residual ibuprofen after 30 minutes of catalytic degradation is less than 10%, compared with the comparative example and other examples. Research shows that the reason for the difference between the different embodiments is that: praseodymium oxide is not formed while carbon nitrogen sintered material forms less active sites when the calcination temperature is 300 deg.c, and carbon nitrogen sintered material is lost more when the calcination temperature is 700 deg.c to result in a decrease in content, thereby lowering the catalytic efficiency.
In conclusion, the prepared in-situ 2, 6-diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous Fenton-like catalyst realizes the successful application of the catalyst in a Fenton-like reaction system, overcomes the defects of the traditional Fenton method, not only enlarges the pH range of the reaction, avoids the formation of iron-containing sludge, but also realizes the synergistic effect of the ferroferric oxide, the praseodymium oxide and a carbon and nitrogen sintering material, accelerates the reaction, can permanently and efficiently remove organic pollutants which are difficult to biodegrade in water, realizes the recycling of the catalyst and is difficult to cause secondary pollution.
Claims (10)
1. The diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous catalyst is characterized in that: comprises ferroferric oxide and sintered praseodymium oxide and diaminopyridine loaded on the ferroferric oxide.
2. A diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous catalyst as claimed in claim 1, characterised in that: the praseodymium oxide and diaminopyridine sinter is obtained by loading praseodymium salt and diaminopyridine on ferroferric oxide and then calcining.
3. A diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous catalyst as claimed in claim 2, characterised in that: the temperature of calcination was 500 ℃.
4. A diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous catalyst as claimed in claim 1, characterised in that: the mass fraction of ferroferric oxide is 62.5%, the mass fraction of praseodymium oxide is 31.25%, and the mass fraction of the diaminopyridine sinter is 6.25%.
5. The use of diaminopyridine sinter praseodymium oxide and ferroferric oxide heterogeneous catalysts as claimed in claim 1, wherein: step one, adding an oxidant into the ibuprofen wastewater;
and step two, adding the diaminopyridine sinter compound praseodymium oxide and ferroferric oxide heterogeneous catalyst into the carbamazepine wastewater to decompose the ibuprofen.
6. The use of diaminopyridine sinter praseodymium oxide and ferroferric oxide heterogeneous catalysts as claimed in claim 5, wherein: in the first step and the second step, the ibuprofen wastewater is continuously stirred; the oxidant in the step one is sodium persulfate; in the second step, the carbamazepine wastewater is kept at 20-30 ℃ for reaction.
7. The method for preparing the diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous catalyst in situ as claimed in claim 1, wherein the method comprises the following steps: step one, adding ferroferric oxide powder into a praseodymium nitrate and diaminopyridine mixed solution, and soaking until the solution is dried to obtain precursor powder;
step two, calcining the precursor powder; calcining and cooling to obtain the diaminopyridine sinter compound praseodymium oxide and ferroferric oxide heterogeneous catalyst.
8. The in-situ preparation method of diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous catalyst according to claim 7, characterized by comprising the following steps: in the first step, the impregnation is carried out under the condition of 80 ℃ water bath.
9. The in-situ preparation method of diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous catalyst according to claim 7, characterized by comprising the following steps: the temperature rise speed of the calcination is 3 ℃ per minute, and the calcination temperature is 300-700 ℃; the calcination time was 3 hours.
10. The in-situ preparation method of diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous catalyst according to claim 7, characterized by comprising the following steps: the preparation process of the ferroferric oxide powder in the first step is as follows: FeSO (ferric oxide) is added4·7H2O and FeCl3·6H2Preheating the mixed solution of O to a preset temperature, and dropwise adding the mixed solution of O into an ammonia water solution subjected to water bath ultrasonic treatment at the preset temperature; after titration, continuously maintaining the mixture at a preset temperature for water bath ultrasonic treatment; and then naturally cooling the mixture to room temperature, centrifugally washing, drying the obtained catalyst, and grinding to obtain ferroferric oxide powder.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202010817724.0A CN112058295B (en) | 2020-08-14 | 2020-08-14 | Diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous catalyst, application thereof and in-situ preparation method |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202010817724.0A CN112058295B (en) | 2020-08-14 | 2020-08-14 | Diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous catalyst, application thereof and in-situ preparation method |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN112058295A true CN112058295A (en) | 2020-12-11 |
| CN112058295B CN112058295B (en) | 2022-12-09 |
Family
ID=73661674
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN202010817724.0A Active CN112058295B (en) | 2020-08-14 | 2020-08-14 | Diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous catalyst, application thereof and in-situ preparation method |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN112058295B (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113289682A (en) * | 2021-06-08 | 2021-08-24 | 中国矿业大学 | CuFe2S3Preparation method and application of (poly) diaminopyridine three-dimensional composite catalyst |
Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS57205325A (en) * | 1981-06-12 | 1982-12-16 | Matsushita Electric Ind Co Ltd | Manufacture of gamma type ferric oxide |
| CN102407128A (en) * | 2011-09-21 | 2012-04-11 | 青岛农业大学 | Preparation method and application of Gd, Pr or Yb doped fenton catalyst |
| CN106140300A (en) * | 2016-07-12 | 2016-11-23 | 河海大学 | Preparation method of one kind fenton catalyst and products thereof and application |
| CN106824205A (en) * | 2017-03-10 | 2017-06-13 | 中触媒新材料股份有限公司 | A kind of application of nickel-base amorphous catalyst and preparation method thereof and catalytic pyridine class compound hydrogenation reaction |
| CN107149946A (en) * | 2017-04-25 | 2017-09-12 | 河南农业大学 | A kind of application of fenton catalyst in degraded organic pollutants |
| CN111268784A (en) * | 2020-03-05 | 2020-06-12 | 浙江工业大学 | Method for treating organic wastewater by multiphase Fenton-like system |
-
2020
- 2020-08-14 CN CN202010817724.0A patent/CN112058295B/en active Active
Patent Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS57205325A (en) * | 1981-06-12 | 1982-12-16 | Matsushita Electric Ind Co Ltd | Manufacture of gamma type ferric oxide |
| CN102407128A (en) * | 2011-09-21 | 2012-04-11 | 青岛农业大学 | Preparation method and application of Gd, Pr or Yb doped fenton catalyst |
| CN106140300A (en) * | 2016-07-12 | 2016-11-23 | 河海大学 | Preparation method of one kind fenton catalyst and products thereof and application |
| CN106824205A (en) * | 2017-03-10 | 2017-06-13 | 中触媒新材料股份有限公司 | A kind of application of nickel-base amorphous catalyst and preparation method thereof and catalytic pyridine class compound hydrogenation reaction |
| CN107149946A (en) * | 2017-04-25 | 2017-09-12 | 河南农业大学 | A kind of application of fenton catalyst in degraded organic pollutants |
| CN111268784A (en) * | 2020-03-05 | 2020-06-12 | 浙江工业大学 | Method for treating organic wastewater by multiphase Fenton-like system |
Non-Patent Citations (2)
| Title |
|---|
| JUNLIANG WANG ET AL.: "Magnetic Pr6O11/SiO2@Fe3O4 particles as the heterogeneous catalyst for the catalytic ozonation of acetochlor: Performance and aquatic toxicity", 《SEPARATION AND PURIFICATION TECHNOLOGY》 * |
| LU HUANG ET AL.: "Immobilized hybrids between nitrogen-doped carbon and stainless steel derived Fe3O4 used as a heterogeneous activator of persulfate during the treatment of aqueous carbamazepine", 《CHEMICAL ENGINEERING JOURNAL》 * |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113289682A (en) * | 2021-06-08 | 2021-08-24 | 中国矿业大学 | CuFe2S3Preparation method and application of (poly) diaminopyridine three-dimensional composite catalyst |
Also Published As
| Publication number | Publication date |
|---|---|
| CN112058295B (en) | 2022-12-09 |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| US20190240646A1 (en) | Mesoporous manganese ferrite fenton-like catalyst, preparation method therefor, and application thereof | |
| CN111790422B (en) | Graphitized nitrogen-complexed Fe (III) -Fe0Catalyst, and synthesis method and application thereof | |
| CN106957438B (en) | Preparation of modified MIL-53(Fe) metal organic framework and method for treating organic wastewater by activating persulfate | |
| CN108940335B (en) | Advanced redox water treatment method based on nitrogen-doped nuclear shell structure magnetic field recoverable iron-carbon material | |
| CN106807376B (en) | Magnetic nano composite catalyst and preparation method and application thereof | |
| CN108097261B (en) | Efficient and stable iron-manganese composite oxide catalyst and preparation method and application thereof | |
| CN109603883A (en) | A kind of@nanometers of phosphatization cobalt composite catalysts of N doping porous carbon polyhedron and preparation method thereof that can efficiently activate persulfate | |
| CN110841654B (en) | Zero-valent iron-loaded iron-manganese oxide composite material, and preparation method and application thereof | |
| CN102145293A (en) | Soft magnetic composite photocatalyst and preparation method thereof | |
| CN113333007B (en) | Nitrogen-doped cobalt iron/carbon catalyst capable of efficiently activating persulfate and preparation method and application thereof | |
| CN115445620B (en) | Preparation method and application of leaf-based biochar supported cobalt-nickel binary metal catalyst | |
| CN112058295B (en) | Diaminopyridine sinter composite praseodymium oxide and ferroferric oxide heterogeneous catalyst, application thereof and in-situ preparation method | |
| CN113426455B (en) | Fenton-like catalyst with manganese dioxide clusters loaded with iron and preparation method thereof | |
| Luo et al. | Graphite phase carbon nitride photo-fenton catalyst and its photocatalytic degradation performance for organic wastewater | |
| CN113731416A (en) | Local acid site modified monatomic catalyst, preparation method and application thereof | |
| CN113318793A (en) | Novel material for producing hydrogen peroxide and removing pollutants, and preparation method and application thereof | |
| CN115445645B (en) | Cu 2+1 O@MXene Fenton catalyst and preparation method and application thereof | |
| CN115814829B (en) | Co and Mo2C-codoped biochar-based composite material and preparation method and application thereof | |
| CN111530451A (en) | GAC-MnO2Nanoparticle composite materials, their preparation and use | |
| CN114950432B (en) | Iron/nitrogen doped carbon-based catalyst with three-dimensional hollow structure, and preparation method and application thereof | |
| CN113171777B (en) | Iron/cerium bimetallic heterogeneous electro-Fenton catalyst and preparation method and application thereof | |
| CN113842942A (en) | Preparation and application of Fe-Ce-LDH/13X granular catalyst for heterogeneous electro-Fenton system | |
| Zhao et al. | Significantly improved H2O2 utilization efficiency over CuFeO2 Fenton-like catalyst through elevating Lewis acidity | |
| CN114130401B (en) | Copper-lanthanum co-modified aluminum-based catalyst and preparation method thereof | |
| Luo et al. | Fe-Cu Bimetallic Oxide Quantum Dots Coupled with gC 3 N 4 Nanosheets for Efficient Photo-Fenton Degradation of Phenol |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| PB01 | Publication | ||
| PB01 | Publication | ||
| SE01 | Entry into force of request for substantive examination | ||
| SE01 | Entry into force of request for substantive examination | ||
| GR01 | Patent grant | ||
| GR01 | Patent grant |