CN111196623A - Novel water vortex-piezoelectric self-driven sewage treatment micro-reactor and treatment method thereof - Google Patents
Novel water vortex-piezoelectric self-driven sewage treatment micro-reactor and treatment method thereof Download PDFInfo
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- 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
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
- C02F1/467—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction
- C02F1/4672—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction by electrooxydation
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- 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
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
- C02F1/467—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction
- C02F1/4676—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction by electroreduction
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- 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
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/469—Treatment of water, waste water, or sewage by electrochemical methods by electrochemical separation, e.g. by electro-osmosis, electrodialysis, electrophoresis
- C02F1/4691—Capacitive deionisation
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- 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
- C02F2101/34—Organic compounds containing oxygen
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- 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
- C02F2101/36—Organic compounds containing halogen
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- 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
- C02F2101/38—Organic compounds containing nitrogen
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- 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
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Abstract
The invention discloses a novel water vortex-piezoelectric self-driven sewage treatment microreactor and a treatment method thereof. The sewage treatment method includes the following steps S1: preparing a pollutant solution, weighing a piezoelectric catalytic material and uniformly mixing the piezoelectric catalytic material with the pollutant solution; s2: pouring the mixed solution into a spiral coil pipe from a water inlet and liquid storage funnel; s3: the entire mixed liquid is received at the water outlet, and step S2 is repeated a plurality of times. The reactor has the advantages of simple structure, convenient operation, low cost, and low maintenance cost and subsequent management cost. The invention does not need external energy supply, only drives the two-dimensional piezoelectric catalytic reaction to degrade pollutants by mechanical force generated by the liquid flowing in the spiral coil, and fully applies the weak water flow machinery which is visible everywhere in the nature to the field of environmental management, thereby avoiding waste.
Description
Technical Field
The invention relates to the technical field of chemical reaction experimental equipment, in particular to a novel water vortex-piezoelectric self-driven sewage treatment micro-reactor utilizing a piezoelectric effect and a treatment method thereof.
Background
With the gradual exhaustion of fossil energy, green, clean and pollution-free renewable energy resources are more and more emphasized by people, and people are dedicated to exploring more forms of renewable resources. The mechanical energy of water is a typical representative of renewable resources, and is found everywhere in natural environment, but they are distributed dispersedly, have small density and low frequency, so that collecting, converting and utilizing the mechanical energy of water is a problem with great significance and great challenge.
In recent years, piezoelectric materials such as zinc oxide (ZnO), an odd number of layers of molybdenum disulfide (MoS)2) Nanosheets, barium titanate (BaTiO)3) Etc., by applying mechanical stress thereto (e.g., ultrasound, agitation, wind, water flow, friction, squeezing, etc.) so that polarization occurs inside the piezoelectric material, electrons and holes are generated. At present, the piezoelectric material is gradually applied to the environmental management and the repair technology. In 2015, wangzhong forest team provided a windmill type air purification system, which takes natural wind as power to drive a windmill to rotate SO as to convert mechanical energy into electric energy, electrically adsorb dust and remove SO2. Self-powered equipment which controls water pollution by taking water flow as a driving force has not been reported for a while, and is yet to be developed.
Disclosure of Invention
The invention aims to overcome the defects and shortcomings of the prior art, and provides a novel water vortex-piezoelectric self-driven sewage treatment micro-reactor which is simple in structure and capable of simulating water flow in a real environment.
The invention also aims to provide a method for treating sewage by using the novel water vortex-piezoelectric self-driven sewage treatment microreactor, wherein a two-dimensional piezoelectric catalytic material is deformed in a reactor to generate piezoelectric charges, and the piezoelectric charges are further combined with oxygen, water and the like to generate a plurality of high-activity free radical components, so that the purpose of catalytically degrading pollutants is achieved.
The purpose of the invention can be realized by the following technical scheme: novel water vortex-piezoelectricity self-driven sewage treatment micro-reactor, including spiral coil and the stock solution funnel of intaking, spiral coil is spiral helicine hollow tube, including water inlet and delivery port water inlet department or water inlet vicinity are equipped with the stock solution funnel of intaking. The reactor can simulate water flow in a real environment.
Preferably, the spiral coil has an inner diameter of 8mm, an outer diameter of 10mm, and a spiral rising angle of 20 °.
As a preferred technical scheme, the total length of the spiral coil is 3m, and the height of the spiral coil is 1 m.
As a preferable technical scheme, a water stop valve is arranged in the water inlet and liquid storage funnel. With this configuration, the stop valve controls the flow of liquid in the funnel.
The other purpose of the invention can be realized by the following technical scheme: the method for treating sewage by using the novel water vortex-piezoelectric self-driven sewage treatment microreactor comprises the following steps: s1: preparing a pollutant solution, weighing a piezoelectric catalytic material and uniformly mixing the piezoelectric catalytic material with the pollutant solution; s2: pouring the mixed solution into a spiral coil pipe from a water inlet and liquid storage funnel; s3: the entire mixed liquid is received at the water outlet, and step S2 is repeated a plurality of times.
Preferably, the piezoelectric catalytic material is a two-dimensional piezoelectric catalytic material.
As a preferred technical scheme, the two-dimensional piezoelectric catalytic material is an odd-number layer of molybdenum disulfide nanosheets, zinc oxide nanosheets or barium titanate nanosheets.
As a preferable technical scheme, the pollutants are rhodamine B, methyl orange, methylene blue, enrofloxacin, ciprofloxacin, metronidazole, benzothiazole or benzotriazole.
As a preferable technical solution, when the contaminant solution is prepared in step S1, water under actual water environmental conditions is used as a background substrate.
As a preferred technical scheme, the background matrix is deionized water, rainwater, river water, tap water or pharmaceutical factory wastewater.
The principle of the invention is as follows: the reactor simulates water flow in a real environment, the two-dimensional piezoelectric catalytic material deforms in the spiral coil pipe through the gravity of the two-dimensional piezoelectric catalytic material and the impact force of the water flow to generate piezoelectric charges, and the piezoelectric charges further react with dissolved oxygen, water and the like in water to generate strong oxygen groups such as hydroxyl radicals and singlet oxygen, so that the piezoelectric charges and pollutants in the water undergo redox reaction to degrade the pollutants. By utilizing the advantages of high-efficiency piezoelectric response of odd-number layers of molybdenum disulfide nanosheets and the like and the characteristic of spontaneous and continuous flow of natural water, the piezoelectric catalyst fully collects the mechanical force generated in the flow process of the natural water to generate strain, and the piezoelectric effect drives the mechanical energy to be converted into electric energy, so that the piezoelectric catalyst directly acts on water pollutants to degrade the water pollutants, and the self-driven self-powered water treatment reaction process of the environment to be taken and used is really realized.
Compared with the prior art, the invention has the following advantages and beneficial effects:
1. the reactor has the advantages of simple structure, convenient operation, low cost, and low maintenance cost and subsequent management cost.
2. The invention does not need external energy supply, only drives the piezoelectric catalytic reaction to degrade pollutants by the mechanical force generated by the liquid flowing in the spiral coil, and fully applies the weak water flow machinery which is visible anywhere in the nature to the field of environmental management, thereby avoiding the waste of the water flow machinery.
3. The reactor and the treatment method thereof have wide application range and are suitable for wastewater treatment under various conditions.
4. The two-dimensional piezoelectric catalytic material adopted by the invention has larger specific surface area, and water pollutants are easily adsorbed by the two-dimensional piezoelectric catalytic material and are further rapidly degraded.
Drawings
FIG. 1 is a schematic view of the structure of a reactor in the example of the present invention;
FIG. 2 is a transmission electron microscope image of an odd number of layers of molybdenum disulfide according to an embodiment of the present invention;
FIG. 3 is a graph showing the effect of degradation of contaminants in a reactor according to an embodiment of the present invention;
FIG. 4 is a graph of the efficiency of degradation of BTH in different reaction systems in examples of the present invention;
FIG. 5 is a graph showing the efficiency of BTH degradation in a water body in practice according to an embodiment of the present invention;
FIG. 6 is a graph showing the effect of different kinds of piezoelectric catalysts on the degradation of MTZ in the examples of the present invention.
Wherein: 1: spiral coil, 2: liquid storage funnel of intaking, 3: water outlet, 4: a water inlet.
Detailed Description
The present invention will be described in further detail with reference to examples and drawings, but the present invention is not limited thereto.
As shown in figure 1, the novel water vortex-piezoelectric self-driven sewage treatment micro-reactor comprises a spiral coil and a water inlet and storage funnel. The spiral coil is a spiral hollow pipe and comprises a water inlet and a water outlet, and a water inlet and liquid storage funnel is arranged at the water inlet or the vicinity of the water inlet. In this embodiment, in order to facilitate the connection of other pipelines at the water inlet, the water inlet liquid storage funnel is arranged at the lower end of the water inlet.
In the embodiment, the inner diameter of the main body of the spiral coil is 8mm, the outer diameter of the main body of the spiral coil is 10mm, the spiral rising angle is 20 degrees, the total length of the coil is 3m, and the height of the coil is about 1 m. A water stop valve is arranged in the water inlet and liquid storage funnel and can control the flow of liquid.
The piezoelectric material used in this embodiment is a two-dimensional sheet, and the molybdenum disulfide is an odd number of layers, i.e., 1, 3, 5, and 7 layers, and the shape thereof is shown in the transmission electron microscope image of fig. 2. The specific synthesis method comprises the following steps: 7 mmole of sodium molybdate (Na)2MoO4·2H2O) and 35 mmol of thiourea were dissolved in 40ml of deionized water, the pH was adjusted to 1 or less with a hydrochloric acid solution having a concentration of 2 mol/l, stirred for one hour, and then the solution was put into a 50 ml-volume reaction tank, and the temperature was maintained atAnd keeping the temperature at 200 ℃ for 24 hours, cooling to room temperature, washing with water, centrifuging, and drying in vacuum to obtain the molybdenum disulfide sample with odd layers.
Example one
In this embodiment, an odd number of molybdenum disulfide nanosheets (MoS) are selected2) The pollutants are respectively selected from rhodamine B (RhB), Methyl Orange (MO) and Methylene Blue (MB) as representatives of dyes, and Enrofloxacin (ENR), Ciprofloxacin (CIP), Metronidazole (MTZ), Benzothiazole (BTH) and Benzotriazole (BTR) as representatives of novel pollutants, and the experiment of degrading the pollutants by using the water flow driven catalyst is carried out in the reactor. In addition, because the flow of water in nature exists and is endless, in the experiment, the flow condition of an actual water body is simulated by circulating water for many times, so that the final treatment effects of different sewage are researched, and an effective scheme is provided for sewage purification in an actual environment.
The experimental procedure was as follows:
s1: preparing a solution of the pollutants, wherein the concentration of the solution is 10 mg/L; weigh 0.020gMoS2And 40mL of contaminant solution.
S2: and pouring the mixed solution into the spiral coil pipe from the water inlet and storage funnel, and allowing the water and the catalyst to flow to the water outlet from top to bottom through the spiral coil pipe.
S3: after all the liquid in the reactor is received at the water outlet, the liquid is poured into the water inlet liquid storage funnel again to flow again, the circulation is carried out for 36 times, samples are taken at intervals of 6 cycles, and the concentration of the pollutants in the liquid is detected.
The degradation effect of each contaminant in the reactor is shown in fig. 3, from which it can be seen that: as the number of cycles increases, the rate of degradation of the contaminants increases. The degradation rate of RhB, MB and ENR after 36 cycles reaches more than 95%; the degradation rate of CIP and MTZ reaches more than 90 percent; BTH and MO also have more than 80% of degradation rate, even if the BTR with stable property and difficult degradation still has 60% of removal rate after 36 cycles in the reactor, which also proves that the reactor of the invention can be applicable to wastewater in various situations. In the process of continuous natural water flow, the environmental water body can realize self-purification under the condition that the water flow drives the piezoelectric catalyst.
Example two
In the embodiment, odd-numbered molybdenum disulfide nanosheets are selected as representatives of high-efficiency piezoelectric catalyst materials, BTH is taken as a representative of novel pollutants, and the characteristics that the materials are subjected to different reaction systems (a system 1: BTH solution + reactor; a system 2: BTH solution + MoS)2Under the condition of standing; system 3: BTH solution + MoS2+ reactor), degradation of contaminants by the reactor.
The specific experimental steps are as follows:
s1: first, a 10mg/L BTH solution was prepared.
S2: for system 1, 40mL of BTH solution was poured into the spiral coil from the inlet reservoir funnel.
S3: after all the liquid in the reactor is received at the water outlet, the liquid is poured into the water inlet liquid storage funnel again, the circulation is carried out for 36 times, samples are taken at intervals of 6 circulation, and the concentration of BTH in the liquid is detected.
For system 2, first 10mg/L BTH solution was prepared, and then 0.020g MoS was weighed2Put into 40mL BTH solution and stand still to ensure no water flow. Samples were taken at intervals (equal in time to the time of circulation in the reactor) to determine the concentration of contaminants in the liquid.
For system 3, first 10mg/L BTH solution was prepared, and then 0.020g MoS was weighed2And after being uniformly mixed with 40mL of BTH solution, the mixed solution is poured into a spiral coil pipe from a water inlet liquid storage funnel, water flow drives a piezoelectric catalyst to flow from top to bottom, all liquid in the reactor is received at a water outlet, and then the mixed solution is poured into the water inlet liquid storage funnel again, the steps are circulated for 36 times, and sampling is carried out at intervals of 6 cycles to detect the concentration of pollutants in the liquid.
The degradation effect of BTH in the different systems is shown in FIG. 4, from which it is apparent that BTH is not substantially degraded in reaction system 1. In reaction system 2, the degradation efficiency of BTH was about 10%. However, in reaction System 3, MoS was observed2The piezoelectric effect is generated, and the degradation of BTHThe efficiency has reached more than 80% already after 24 cycles and 90% after 36 cycles. This also indicates that the degradation of the contaminants in the reactor is catalyzed by the piezoelectric effect of the piezoelectric material driven by the mechanical force of the water current.
EXAMPLE III
In the embodiment, an odd number of layers of molybdenum disulfide nanosheets are selected as a representative of a high-efficiency piezoelectric catalyst material, BTH is taken as a representative of a novel pollutant, water with different actual conditions is taken as a background substrate (respectively deionized water, rainwater, river water, tap water and pharmaceutical factory wastewater), an experiment for degrading the pollutant by using a water flow driven catalyst is carried out in the reactor, so that the degradation condition of the pollutant under the actual water environment condition is researched, and a reference basis is provided for the development of practical application.
The specific experimental steps are as follows:
s1: deionized water, rainwater, saline water (0.9% NaCl solution) and pharmaceutical factory wastewater after standing are respectively taken as solvents to prepare BTH solution with the concentration of 10 mg/L. 0.020g of MoS is weighed2And mixed well with 40mL of BTH solution.
S2: and pouring the mixed solution into the spiral coil pipe from the water inlet and storage funnel, and allowing the water and the catalyst to flow to the water outlet from top to bottom through the spiral coil pipe.
S3: after all the liquid in the reactor is received at the water outlet, the liquid is poured into the water inlet liquid storage funnel again, the circulation is carried out for 36 times, and sampling is carried out at intervals of 6 cycles to detect the concentration of the pollutants in the liquid.
The degradation effect of pollutants in different water qualities is shown in fig. 5, and it can be easily seen from the graph that after 36 cycles of experiments, the degradation effect of the BTH solution using deionized water as a solvent reaches 90%, and the BTH solution using saline water, rainwater and pharmaceutical factory wastewater with complex components as a solvent still has about 70% of degradation efficiency after 36 cycles in the reactor. The method can be expected to completely degrade pollutants under the driving of continuous water flow in the nature, and fully embody the water body purification. This demonstrates the general applicability and effectiveness of the reactor of the present invention, meeting the conditions for degrading various refractory wastewater in some industries; has great practical application potential.
Example four
In this example, MTZ was chosen as representative of the contaminants, and MoS was compared in the reactor2ZnO and BaTiO3The three common piezoelectric materials have the effect of degrading contaminants.
The specific experimental steps are as follows:
s1: firstly, preparing 10mg/L MTZ solution; 0.02mg of MoS was weighed out separately2ZnO and BaTiO3And uniformly mixing the MTZ solution prepared in the step 40mLS 1.
S2: the mixed solution was poured from the reactor's influent receiver funnel into the coil.
S3: after all the liquid in the reactor is received at the water outlet, the liquid is poured into the water inlet liquid storage funnel again, the circulation is carried out for 36 times, and sampling is carried out at intervals of 6 cycles to detect the concentration of the pollutants in the liquid.
The degradation effect of MTZ in a reactor with different piezoelectric materials as catalysts is shown in FIG. 6, which shows: the degradation efficiency of MTZ gradually increases with the number of cycles. After 36 cycles, at MoS2The degradation efficiency of the reaction system MTZ as a catalyst is about 90 percent; BaTiO 23The next, about 70%; finally ZnO, the degradation efficiency is about 50 percent. This also reflects the general adaptability of the reactor to piezoelectric materials, which can produce a certain piezoelectric effect for different piezoelectric catalysts. Provides a reliable method for industrial treatment of wastewater.
The above-mentioned embodiments only express several embodiments of the present invention, and the description thereof is more specific and detailed, but not construed as limiting the scope of the present invention. It should be noted that, for a person skilled in the art, several variations and modifications can be made without departing from the inventive concept, which falls within the scope of the present invention. Therefore, the protection scope of the present patent shall be subject to the appended claims.
Claims (10)
1. Novel water vortex-piezoelectricity self-driven sewage treatment micro-reactor, its characterized in that, including spiral coil and the stock solution funnel of intaking, spiral coil is spiral helicine hollow tube, including water inlet and delivery port water inlet department or water inlet vicinity are equipped with the stock solution funnel of intaking.
2. The reactor according to claim 1, wherein the helical coil has an inner diameter of 8mm, an outer diameter of 10mm, and a helix angle of 20 °.
3. The reactor according to claim 2, wherein the helical coil has a total length of 3m and a height of 1 m.
4. The reactor of claim 1, wherein a water stop valve is disposed in the water inlet and storage funnel.
5. A method for treating wastewater using the reactor according to any one of claims 1 to 4, comprising the steps of:
s1: preparing a pollutant solution, weighing a piezoelectric catalytic material and uniformly mixing the piezoelectric catalytic material with the pollutant solution;
s2: pouring the mixed solution into a spiral coil pipe from a water inlet and liquid storage funnel;
s3: the entire mixed liquid is received at the water outlet, and step S2 is repeated a plurality of times.
6. The process of claim 5, wherein the piezoelectric catalytic material is a two-dimensional piezoelectric catalytic material.
7. The treatment method according to claim 6, wherein the two-dimensional piezoelectric catalytic material is an odd number of layers of molybdenum disulfide nanosheets, zinc oxide nanosheets, or barium titanate nanosheets.
8. The treatment method of claim 5, wherein the contaminant is rhodamine B, methyl orange, methylene blue, enrofloxacin, ciprofloxacin, metronidazole, benzothiazole, or benzotriazole.
9. The treatment method as claimed in claim 5, wherein water under actual aquatic environmental conditions is used as a background substrate when the contaminant solution is prepared in step S1.
10. The treatment method of claim 8, wherein the background substrate is deionized water, rainwater, river water, tap water, or pharmaceutical factory wastewater.
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| CN114057257A (en) * | 2021-11-18 | 2022-02-18 | 河海大学 | Piezoelectric-photocatalytic pollutant degradation device based on hydroelectric power generation |
| CN114590868A (en) * | 2022-03-24 | 2022-06-07 | 河海大学 | Spiral piezoelectric photocatalytic sewage treatment device and treatment method |
| CN114634242A (en) * | 2022-03-29 | 2022-06-17 | 河海大学 | Water pollutant degradation aeration integrated device based on piezoelectric catalysis |
| CN114804299A (en) * | 2022-06-10 | 2022-07-29 | 青岛科技大学 | Preparation of flexible piezoelectric liner tube and application of flexible piezoelectric liner tube in self-driven degradation of organic pollutants |
| WO2022167915A1 (en) * | 2021-02-02 | 2022-08-11 | Oxyle Ag | Assemblies and methods for treating polluted water |
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| CN114804299A (en) * | 2022-06-10 | 2022-07-29 | 青岛科技大学 | Preparation of flexible piezoelectric liner tube and application of flexible piezoelectric liner tube in self-driven degradation of organic pollutants |
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| CN111196623B (en) | 2022-04-29 |
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