CN111389425B - Perovskite photocatalytic material for removing algae in water body and preparation method thereof - Google Patents
Perovskite photocatalytic material for removing algae in water body and preparation method thereof Download PDFInfo
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- 239000000463 material Substances 0.000 title claims abstract description 25
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- 238000002360 preparation method Methods 0.000 title claims abstract description 6
- 229910017771 LaFeO Inorganic materials 0.000 claims abstract description 30
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- HKZLPVFGJNLROG-UHFFFAOYSA-M silver monochloride Chemical compound [Cl-].[Ag+] HKZLPVFGJNLROG-UHFFFAOYSA-M 0.000 claims abstract description 21
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 claims description 20
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 claims description 15
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- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 4
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- SQGYOTSLMSWVJD-UHFFFAOYSA-N silver(1+) nitrate Chemical compound [Ag+].[O-]N(=O)=O SQGYOTSLMSWVJD-UHFFFAOYSA-N 0.000 description 4
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 3
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- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 1
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- 229910000365 copper sulfate Inorganic materials 0.000 description 1
- ARUVKPQLZAKDPS-UHFFFAOYSA-L copper(II) sulfate Chemical compound [Cu+2].[O-][S+2]([O-])([O-])[O-] ARUVKPQLZAKDPS-UHFFFAOYSA-L 0.000 description 1
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- MVFCKEFYUDZOCX-UHFFFAOYSA-N iron(2+);dinitrate Chemical compound [Fe+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O MVFCKEFYUDZOCX-UHFFFAOYSA-N 0.000 description 1
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Images
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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
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/06—Halogens; Compounds thereof
- B01J27/128—Halogens; Compounds thereof with iron group metals or platinum group metals
-
- B01J35/39—
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/50—Treatment of water, waste water, or sewage by addition or application of a germicide or by oligodynamic treatment
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2303/00—Specific treatment goals
- C02F2303/04—Disinfection
-
- 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 a perovskite photocatalytic material for removing algae in a water body and a preparation method thereof, which utilize the characteristics of sensitivity of algae to silver and good photoresponse of the perovskite material to prepare AgCl/LaFeO capable of removing algae cells in the water body under visible light 3 A material. The perovskite visible-light-catalyzed material prepared by the invention has the characteristics of high photocatalytic activity and strong bacteriostatic effect, and can be directly added into water to realize photocatalytic degradation of algae cells in water.
Description
Technical Field
The invention belongs to the technical field of water treatment, and particularly relates to a perovskite photocatalytic material for removing eutrophic water algae and a preparation method thereof.
Background
In recent years, as global warming has been progressed, outbreaks of harmful algal blooms have caused serious threats to fishery, tourism, marine ecological environments and human health, and have become one of the global ecological disasters. The mass propagation of algae not only affects the beautiful environment and emits foul smell, but also can kill fishes and other wild animals and plants under the anoxic/hypoxic condition to pollute drinking water sources, and meanwhile, the algal toxin released when the algae die can cause damage to nerves, muscles and livers of human bodies and even die seriously. Therefore, how to effectively control the cyanobacterial bloom becomes a research hotspot in the environmental field.
The existing methods for controlling cyanobacterial bloom mainly comprise a physical method, a chemical method, a biological method and the like. The physical method is to remove algae in water by physical means, and mainly comprises manual mechanical fishing, cell destruction (such as ultrasonic disruption) and the like. The artificial machinery is used for fishing and removing the algae, secondary pollution can not be generated, but more manpower and material resources are needed in the implementation process, the cost is higher, and the artificial machinery can only be used as an emergency measure when the bloom breaks out. The ultrasonic method can destroy algae cells, but at the same time, the contents of the algae cells can leak out, and the change of the taste and the smell of the water body can be caused. The chemical method is generally to kill the cyanobacteria cells directly by the strong oxidizing property (chlorine, ozone, permanganate, etc.) or toxicity (such as copper sulfate) of the reagent, or to remove the cyanobacteria cells after precipitation by flocculation. Chemical methods have quick algae removal effect, but chemical reagents can cause damage to other aquatic organisms and easily cause secondary pollution (such as generation of disinfection byproducts and the like). The biological method mainly controls the growth of blue algae cells and the like through other organisms, such as microbial action, feeding of shellfish and the like, and competition and allelopathy of other phytoplankton and the like. But the biological method has slow effect, less stable effect, great influence by environmental conditions and difficult popularization.
The photocatalytic technology is favored because of its characteristics of environmental friendliness, clean energy, low cost, complete degradation of pollutants and the like, and is gradually applied to the field of environment. However, the existing common photocatalyst still has many defects, which limits the application of the photocatalyst in practical application. If the band gap value is very wide, the ultraviolet light can be excited only under ultraviolet light (lambda is less than 380 nm), and the ultraviolet light only accounts for 2-3% of the solar spectrum, and the defect of low visible light utilization efficiency caused by high electron-hole recombination rate of the generated light is overcome. In recent years, perovskite materials have been used in solar power generation, electrocatalysis, photocatalytic water decomposition, and carbon dioxide (CO) 2 ) Reduction and contaminant removal applications are of interest. Ideal perovskite ABX 3 The structure has cubic symmetry, in which the X anion is usually oxygenIons or halide ions (F, Cl, Br or I), a cations are generally larger than B cations, the nature of the perovskite is determined by the cations occupying its a and B site lattice, and more than 90% of the metal elements can be successfully incorporated into the perovskite lattice. Therefore, the A site and the B site can be replaced by different elements, so that electron spin state coupling is generated between the elements, and the composition of the perovskite is changed, so that the structure of the perovskite is distorted to a certain extent, the structural symmetry and the positions of positive and negative charge centers of the perovskite are changed, and cations or oxygen vacancies are generated, which has important significance for adjusting the energy band structure of the material, separating photogenerated charge carriers and improving the efficiency of the photocatalyst.
The perovskite photocatalytic material also has great potential in the aspect of being applied to algae removal: (1) the perovskite oxide has a narrow band gap and high visible light response, the light response reaction range comprises the whole visible light region, even at 800nm, the perovskite oxide still shows high light absorption, and visible light and ultraviolet light can be simultaneously utilized; (2) part of the iron-based perovskite oxide perovskite material has magnetism and has strong potential in designing a magnetic recyclable photocatalyst; (3) the surface of the microcystis aeruginosa has negative charge of the surface functional group, so that a positively charged perovskite material can be designed, and the effective contact of the photocatalyst and the algae can be increased by utilizing electrostatic adsorption. Therefore, research and development of the perovskite material with visible light catalytic activity can well fill the defects of the photocatalyst in practical application, and further improve the performance of the photocatalyst algae removal technology in the field of blue algae bloom treatment.
Disclosure of Invention
The invention aims to provide a perovskite photocatalytic material for removing algae in a water body and a preparation method thereof, which are used for relieving the problem of cyanobacterial bloom.
In order to achieve the purpose, the invention adopts the following technical scheme:
a perovskite photocatalytic material for removing algae in a water body is prepared by the following steps:
1）LaFeO 3 the synthesis of (2): dissolving ferric nitrate, lanthanum nitrate and citric acid in deionized water, magnetically stirring for 1 h,then transferring the mixture into a stainless steel autoclave lined with teflon, sealing and keeping the autoclave at 180 ℃ for 12 hours, naturally cooling the autoclave to room temperature, centrifugally separating, washing the obtained precipitate with deionized water for 3 times, drying the precipitate with air at 80 ℃ and grinding the dried precipitate into powder, and finally calcining the powder at 800 ℃ for 4 hours to obtain LaFeO 3 Powder;
2）AgCl/LaFeO 3 the synthesis of (2): the obtained LaFeO is subjected to 3 Dissolving the powder in AgNO 3 Stirring the solution for 3 h at room temperature, then dropwise adding the solution into NaCl solution within 20min, stirring for 10 h at room temperature, finally washing with deionized water for three times to remove excessive NaCl, and drying at 70 ℃ for 12 h to obtain AgCl/LaFeO 3 And (3) powder.
Further, the molar ratio of the iron nitrate, the lanthanum nitrate and the citric acid used in the step 1) is 2:2: 5.
Further, AgNO used in step 2) 3 The concentration of the solution was 6.39 mg/mL and the concentration of the NaCl solution was 0.75 mg/mL. The generated AgCl/LaFeO 3 AgCl and LaFeO in powder 3 The mass ratio of (A) to (B) is 1: 1-1: 4.
The perovskite photocatalytic material obtained by the invention is brownish red powder macroscopically and is composed of AgCl and LaFeO microscopically 3 The close combination structure can be used for removing algae in water body.
Compared with the existing algae removal technology, the invention has the following advantages:
1. the invention utilizes the characteristics of sensitivity of algae to silver and good photoresponse of perovskite material to prepare AgCl/LaFeO 3 The photocatalytic material has the characteristics of high photocatalytic activity, capability of being excited under visible light, good bacteriostatic effect and the like.
2. The perovskite photocatalytic material prepared by the invention has positive electricity in water, and the surface of microcystis aeruginosa has negative electricity due to the surface functional group, so that the effective contact of the photocatalyst and algae can be increased by utilizing electrostatic adsorption, and the photocatalytic algae removal effect is improved.
3. The photocatalytic material prepared by the method can be recycled, so that the economic benefit is improved.
Drawings
FIG. 1 is the AgCl/LaFeO prepared in the examples 3 The algae removal effect of the material under visible light is compared with the situation.
Detailed Description
In order to make the present invention more comprehensible, the technical solutions of the present invention are further described below with reference to specific embodiments, but the present invention is not limited thereto.
Examples
（1）LaFeO 3 Synthesis of (2)
0.808 g (2.0 mmol) of Fe (NO) 3 ) 3 ·9H 2 O、0.866 g（2.0 mmol） La(NO 3 ) 3 ·6H 2 Dissolving O and 0.964g (5.0 mmol) of citric acid in 180 mL of deionized water, magnetically stirring for 1 h, transferring to a 200mL stainless steel autoclave lined with Teflon, sealing and keeping at 180 ℃ for 12 h, naturally cooling the autoclave to room temperature, taking the product for centrifugal separation, washing the obtained precipitate with deionized water for 3 times, drying in air at 80 ℃, grinding into powder, and calcining at 800 ℃ for 4 h to obtain LaFeO 3 And (3) powder.
（2）AgCl/LaFeO 3 Synthesis of (2)
0.1278 g (0.75 mmol) AgNO 3 Dissolved in 20mL of deionized water to prepare a silver nitrate solution, and 0.06 g (1.0 mmol) of NaCl was dissolved in 80 mL of deionized water to prepare a sodium chloride solution. 0.2 g of LaFeO was weighed 3 Dissolving in prepared silver nitrate solution, stirring at room temperature for 3 h, adding the solution dropwise into the prepared sodium chloride solution within 20min, stirring at room temperature for 10 h, washing with deionized water for three times to remove excess NaCl, drying at 70 deg.C for 12 h, and grinding into powder to obtain AgCl/LaFeO 3 。
Selecting initial algae density of 6.48 × 10 6 cells/mL microcystis aeruginosa solution is taken as a removal object, and the visible light catalysis AgCl/LaFeO is explored by taking chlorophyll a as an index 3 The algae removal effect. The specific method is to take 5 mg AgCl/LaFeO 3 Adding into 100 mL of algae solution, marking as experimental group, so as not to add AgCl/LaFeO 3 The algae liquid,Separately adding AgCl algae solution and separately adding LaFeO 3 The algal solution was used as a control group. The experimental group and the control group were placed in a photocatalytic reactor (using a cut-off filter to remove ultraviolet light with a wavelength of < 420 nm) for photocatalytic reaction for 180 min, and the chlorophyll a content was measured by sampling every 30 min, and the experimental results are shown in fig. 1.
As can be seen from FIG. 1, in AgCl/LaFeO 3 Under the action, the chlorophyll a content of algae cells is rapidly reduced, and after 150 min of illumination, the removal rate of the chlorophyll a reaches 100 percent without adding AgCl/LaFeO 3 The control group has no response to environmental change and light source effect, the removal rate of chlorophyll a after illumination for 180 min is only 7.1%, and AgCl or LaFeO is added separately 3 The removal rate of chlorophyll a after 180 min of illumination is only 23.1% and 21.5%, respectively.
The above description is only a preferred embodiment of the present invention, and all equivalent changes and modifications made in accordance with the claims of the present invention should be covered by the present invention.
Claims (2)
1. The application of the perovskite photocatalytic material in removing algae in water is characterized in that: the preparation method of the perovskite photocatalytic material comprises the following steps:
1）LaFeO 3 the synthesis of (2): dissolving ferric nitrate, lanthanum nitrate and citric acid in deionized water, magnetically stirring for 1 h, transferring the mixture into a stainless steel autoclave lined with teflon, sealing and keeping at 180 ℃ for 12 h, naturally cooling the autoclave to room temperature, centrifugally separating, washing the obtained precipitate with deionized water for 3 times, drying in air at 80 ℃ and grinding into powder, and finally calcining at 800 ℃ for 4 h to obtain LaFeO 3 Powder;
2）AgCl/LaFeO 3 the synthesis of (2): the obtained LaFeO is subjected to 3 Dissolving the powder in AgNO 3 Stirring the solution for 3 h at room temperature, then dropwise adding the solution into NaCl solution within 20min, stirring for 10 h at room temperature, finally washing with deionized water for three times to remove excessive NaCl, and drying at 70 ℃ for 12 h to obtain AgCl/LaFeO 3 Powder;
AgNO used in step 2) 3 The concentration of the solution is 6.39 mg/mL, and the concentration of the NaCl solution is 0.75 mg/mL; the generated AgCl/LaFeO 3 AgCl and LaFeO in powder 3 The mass ratio of (A) to (B) is 1: 1-1: 4.
2. Use of the perovskite photocatalytic material according to claim 1 for removing algae in a body of water, characterized in that: the molar ratio of the ferric nitrate to the lanthanum nitrate to the citric acid used in the step 1) is 2:2: 5.
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