CN111807477B - Method for removing antibiotic resistance gene based on solar heating film electrolysis - Google Patents
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Abstract
The invention relates to a method for removing antibiotic resistance genes based on solar heating film electrolysis, which comprises an electrolytic cell, wherein the upper part of the electrolytic cell is a platinum wire serving as a cathode, the lower part of the electrolytic cell is a solar heating conductive film serving as an anode, the two electrodes are connected to an external power supply through leads to form a closed loop, the two sides of the upper part of the electrolytic cell are respectively provided with a water inlet and a water outlet, the lower part of the solar heating conductive film is an annular supporting layer, and membrane filter liquid flows out from the annular supporting layer. A sunlight simulator is arranged outside the reactor to simulate sunlight. The invention combines the traditional membrane interception with a chemical electrolytic cell, loads a photo-thermal conversion material on the membrane, and destroys the structure of resistant bacteria and inactivates the resistant genes by utilizing the local high-temperature and acidic environment formed in a reactor, thereby achieving the purpose of removing the resistant genes.
Description
Technical Field
The invention relates to a method for removing antibiotic resistance genes based on solar heating film electrolysis, and belongs to the technical field of sewage purification treatment.
Background
Antibiotics exist widely in natural environment, the types of the antibiotics are various, the antibiotic residual quantity is the highest with the waste water of a farm, and the underground water is the lowest. The current situation of antibiotic pollution in domestic environment is more serious than that in foreign countries. The problem of environmental pollution caused by the heavy use of antibiotics and even abuse of antibiotics is becoming more serious, and the ecological environment safety and human health are seriously threatened by the pollution of Antibiotic Resistance Genes (ARGs) generated by microorganisms in animals induced by the selective pressure of antibiotics or microorganisms induced in the environment after entering the environment. The ARGs can carry out horizontal gene transfer in the same or different flora through movable gene elements such as plasmids, integron-gene cassettes, transposons and the like, have persistence and reproducibility in the environment and are considered as a novel environmental pollutant.
Resistance gene pollution exists in water, soil and atmosphere to different degrees, wherein tetracycline ARGs are detected in different environments. At present, resistance genes exist in basically all sewage plants in China, and resistance genes are also detected in natural water, for example, researches of scholars find that sulfonamides ARGs are the resistance genes with the highest occurrence frequency in water samples and sediments of Jiulongjiang, and tetracyclines ARGs and sulfonamides ARGs are detected in sediment samples. Resistance genes have been treated as environmental pollutants.
The existence form of the resistance gene is two types: present in resistant bacteria, free from the environment, and predominantly in the former. At present, the advanced oxidation process and the disinfection process are mainly used for removing the resistance genes. Advanced oxidation can destroy the double helix structure of bacterial DNA through physical or chemical mutagenesis, thereby effectively reducing the content of the resistance gene in effluent, but the practical application of the advanced oxidation has great limitations, firstly, the cost is high, secondly, the treatment effect is not good, and the resistance gene existing in bacteria can not be effectively removed. Sterilization plays an important role in reducing resistance genes in sewage not only because it can reduce the number of live resistant bacteria but also effectively inhibit gene transfer between live resistant bacteria. The effect of reduced resistance to disinfection depends on the degree of penetration of the disinfectant into the body of the resistant bacteria, and the reactivity of various components (e.g., amino acids, fats, carbohydrates, nucleic acids) within the cell. If the disinfectant causes cell inactivation independent of the nucleic acid, the intact resistance gene fragment remains in the cell and may be transferred to other microorganisms, and thus the disinfection cannot effectively remove the resistance gene.
The membrane interception is a common pollutant removal mode in the water treatment process, and has high treatment efficiency and stable water outlet. The amount of the resistance genes and bacteria in the effluent can be greatly reduced by adopting membrane interception, but the resistance genes and bacteria do not disappear, but exist in the concentrated water on one side of the membrane, the concentration is greatly increased compared with the original concentration, and further treatment is needed. Meanwhile, because the membrane has high cost, membrane pollution is easy to occur, the energy consumption in the operation process is high, and the practical application of membrane interception still has a great limit.
Therefore, there is a need to develop an economical and efficient technique for removing antibiotic resistance genes.
The invention content is as follows:
aiming at the defects of the prior art, the invention provides a method for removing antibiotic resistance genes based on solar heat-generating film electrolysis.
The method combines membrane interception with a chemical electrolytic cell, loads a photo-thermal conversion material capable of conducting electricity on the membrane, inactivates resistant bacteria and destroys a resistant gene structure by utilizing local high temperature and acidic conditions formed in a reactor, so as to achieve the aim of removing the resistant gene, and toxic byproducts are not generated in the process. Meanwhile, the external electric field can effectively reduce membrane pollution, prolong the service life of the membrane and have good economic benefit.
In order to achieve the purpose, the invention is realized by the following technical scheme:
a method for removing antibiotic resistance genes based on solar heating film electrolysis is carried out by utilizing a solar heating film electrolysis system, wherein the solar heating film electrolysis system comprises a sewage container, a water pump and an electrolytic cell which are communicated; a water inlet and a water outlet are respectively arranged on two sides of the upper end of the electrolytic cell, and an anode and a cathode are fixed in the electrolytic cell between the water inlet and the water outlet; the anode and the cathode are respectively connected to the anode and the cathode of an external power supply through metal leads to form an electrolytic cell, and the bottom of the electrolytic cell is provided with a filtrate outlet;
the anode is a solar heating conductive film, the solar heating conductive film is arranged on an annular supporting layer at the bottom of the electrolytic cell, the cathode is a platinum electrode, and the solar heating conductive film is obtained by loading a conductive photo-thermal conversion material on a PVDF ultrafiltration membrane;
the method for removing the antibiotic resistance gene is as follows: the method comprises the following steps of enabling sewage containing antibiotic resistance genes to enter an electrolytic cell through a water inlet, turning on a power supply, illuminating at the same time, enabling a solar heating conductive film to absorb solar energy to generate high temperature on the surface of the film, enabling the antibiotic and resistant bacteria structures flowing to the surface of the film along with water to be damaged, releasing the resistance genes, inactivating the resistance genes under the combined action of the high temperature and acidic conditions, filtering through the solar heating conductive film, and discharging from a filtrate outlet to remove the antibiotic resistance genes.
According to the invention, the solar heating conductive film is prepared by the following steps:
(1) placing the PVDF membrane on a dopamine hydrochloride solution, and standing for 10-20min to obtain an ultrafiltration membrane loaded with a polydopamine layer;
(2) dispersing the photo-thermal conductive material into a polyvinyl alcohol (PVA) solution to obtain a photo-thermal conductive material-PVA solution, and carrying out pressure deposition or electrostatic spinning on the photo-thermal conductive material-PVA solution onto the poly dopamine layer-loaded ultrafiltration membrane in the step (1) to form a PVA nanofiber network containing the photo-thermal conductive material, so as to obtain the solar heating conductive film.
Preferably, in step (1), the concentration of the dopamine hydrochloride solution is 1-5mg/mL, and the pH value is 8.5.
Preferably, in the step (2), when the pressure deposition method is adopted, the mass ratio of the photothermal conductive material to the polyvinyl alcohol (PVA) in the photothermal conductive material-polyvinyl alcohol solution is 1: 2 to 6, the pressure during pressure deposition is 0.1MPa, and the deposition time is 1 h.
Preferably, in the step (2), when the electrostatic spinning mode is adopted, the concentration of the photothermal conductive material in the photothermal conductive material-polyvinyl alcohol solution is 3-6wt%, the distance between the injector and the metal plate is 10cm, the injection rate of the injector is 0.5mL/min, the voltage is 10kV, and the spinning time is 3 h.
According to the present invention, preferably, the photothermal conductive material is Carbon Nanotubes (CNTs), carbon black, graphene or doped gold nanoparticles.
Most preferably, the photothermal conductive material is Carbon Nanotubes (CNTs).
According to the present invention, in the method for removing the antibiotic resistance gene, the distance between the solar heat conductive film and the platinum electrode is preferably 3 to 6 cm.
In the method for removing antibiotic resistance gene according to the present invention, the voltage of the power source is 1-3V and the intensity of the light is 1-3kw/m2。
According to the preferable method for removing the antibiotic resistance gene, the sewage is secondary effluent of a sewage treatment plant, livestock wastewater, breeding wastewater, pharmaceutical wastewater or medical wastewater.
In the operation process of the method for removing the antibiotic resistance gene, the anode generates oxidation reaction to enrich hydrogen ions to form a local acid environment, and the unwinding and hydrolysis of the resistance gene can be accelerated by combining a high-temperature environment generated on the surface of the solar heating conductive film, so that the harmlessness of the resistance gene is realized.
According to the solar heating conductive film disclosed by the invention, when sunlight irradiates, the CNT absorbs solar energy and converts the solar energy into heat energy, and local high temperature is generated on the surface of the film. In the water treatment process, the resistant bacteria and the resistant genes reach the surface of the membrane along with water flow, the structure of the bacteria is destroyed and the resistant genes are released under the action of local high temperature, the double helix structure of the genes is opened, the resistant genes are released, the resistant genes are inactivated under the combined action of high temperature and acid conditions and no longer have resistance, and the resistant bacteria and the like in the sewage are intercepted on the surface of the membrane, so that the treatment time is prolonged. After a series of treatments, the membrane filtrate basically does not contain resistance genes, and the inlet water exceeding the membrane interception capacity is discharged from the water outlet and flows back to the water inlet.
The invention adopts a commercial PVDF ultrafiltration membrane which can resist high temperature, can intercept bacteria, large gene fragments and other particulate matters, suspended matters and macromolecular organic pollutants in water, and can ensure the quality of the effluent water on one hand; on the other hand, the pollutants are trapped on the surface of the membrane, so that the contact time with high-temperature and acidic environment is prolonged, and the removal effect is enhanced.
The invention has the advantages that:
1. the pollutants and the resistance genes are trapped on the surface of the membrane, so that the effluent quality can be ensured, the treatment time of the resistance genes can be prolonged, and the removal effect is improved.
2. The solar heating conductive film is adopted, and the photo-thermal conversion material is loaded, so that the ultrafiltration membrane can generate local high temperature under the action of solar energy, can sterilize and destroy a DNA double helix structure, is low in energy consumption and high in efficiency, and cannot generate toxic byproducts under the action of high temperature.
3. The membrane electrode is used as an anode, and when the membrane electrode is electrified, a local acidic environment is generated on the surface of the membrane and is coupled with a high-temperature environment, so that the hydrolysis of the secondary structure of the resistance gene can be accelerated, and the removal of the resistance gene is strengthened.
4. The cathode is subjected to reduction reaction to generate hydrogen, so that clean energy can be provided, the electricity of the electrolytic cell can be supplemented, and the energy conservation and environmental protection are realized.
5. The solar heating conductive film and the electrolytic cell are combined and mutually promoted, so that the treatment effect can be effectively improved. The loaded CNT material can endow the film with conductivity while carrying out photo-thermal conversion, and the external electric field can obviously reduce the film pollution, improve the film flux and prolong the service life of the film.
Description of the drawings:
FIG. 1 is a schematic structural view of a solar heating film electrolysis system of the present invention
In the figure: 1. a water inlet; 2. a platinum wire; 3. a water outlet; 4. a solar heating conductive film; 5. a ring-shaped supporting layer; 6. a filtrate outlet; 7. a wire; 8. a power source; 9. a water pump; 10. a sewage container; 11. a solar simulator; 12. an electrolytic cell.
The specific implementation mode is as follows:
the following is further described with reference to the drawings and examples, but is not limited thereto.
Example 1:
the structure of the solar heating film electrolysis system is shown in figure 1, and the solar heating film electrolysis system comprises a water pump and an electrolytic cell 12 which are communicated; the upper end of the electrolytic cell 12 is provided with a water inlet 1 and a water outlet 3 at two sides respectively, and an anode and a cathode are fixed in the electrolytic cell between the water inlet 1 and the water outlet 3; the anode is a solar heating conductive film 4, the solar heating conductive film is arranged on an annular supporting layer 5 at the bottom of the electrolytic cell, the cathode is a platinum electrode 2, the platinum electrode 2 is directly connected with a lead 7 to the cathode of an external power supply 8, two sides of the solar heating conductive film electrode 4 are connected to the anode of the power supply 8 through leads to form the electrolytic cell, and the bottom of the electrolytic cell is provided with a filtrate outlet 6; the secondary effluent of the sewage treatment plant in the sewage container 10 is lifted to the water inlet 1 by the water pump 9, and the sewage exceeding the membrane filtration capacity is discharged from the water outlet 3 and returns to the sewage container 10 again. The reactor is externally provided with a short-arc xenon lamp sunlight simulator 11 for simulating the irradiation of sunlight and providing solar energy.
The method for removing the antibiotic resistance gene is as follows: the sewage containing the antibiotic resistance genes enters the electrolytic cell through the water inlet, the power supply is turned on, meanwhile, illumination is carried out, the solar heating conductive film absorbs solar energy to generate high temperature on the surface of the film, the antibiotic and resistant bacteria structures flowing to the surface of the film along with water are damaged, the resistance genes are released, the resistance genes are inactivated under the combined action of the high temperature and the acidic condition, and the sewage is filtered by the solar heating conductive film and then is discharged from a filtrate outlet to remove the antibiotic resistance genes.
The solar heating conductive film is prepared by the following method:
(1) one side of the PVDF membrane is contacted with 1-5mg/mL dopamine hydrochloride solution with pH of 8.5 for 10-20min, and the polydopamine layer can assist in adhering the hydrophilic photothermal layer on the hydrophobic PVDF membrane.
(2) Fixing the carbon nano tube: the CNTs are dispersed into the PVA solution, pre-treated with polydopamine to ensure adhesion, and the PVA-CNT solution is pressure deposited or electrospun onto the PVDF membrane to form a PVA nanofiber network containing CNTs.
Experimental example 1:
the secondary effluent of a certain sewage treatment plant is treated by using the solar heating membrane electrolytic cell in the embodiment 1, and six genes are selected: sulfanilamide resistance genes sulI and sulI, tetracycline resistance genes tetA and tetW, class I integron integrase genes int I and 16S rRNA, and the initial abundance of the sulfanilamide resistance genes sulI and the tetracycline resistance genes tetA and tetW are respectively 1.93 multiplied by 105～9.95×106copies/mL、2.34×108～4.26×108copies/mL、7.64×107～9.22×107copies/mL、1.37×107～6.19×107copies/mL、4.37×107～9.15×107copies/mL、3.42×108～3.72×109copies/mL were treated with a PVDF film not carrying a photothermal conversion material and a modified solar heat conductive film, respectively, and the concentrations of the six genes after the treatment were measured, and the results are shown in Table 1.
Table 1: removal of resistance genes from PVDF film and solar heat-generating conductive film
Experimental example 2:
the solar heating membrane electrolytic cell in example 1 is used for treating breeding wastewater of a certain pig farm, and six genes are selected: sulfanilamide resistance genes sul I and sul II, tetracycline resistance genes tetM, tet W, tet Q and I type integrase gene int I, and the results are shown in a table 2 by comparing the absolute abundance of the water inlet and outlet resistance genes.
Table 2: removal of resistance gene of solar heating membrane electrolytic cell to breeding wastewater
From the experimental results, the method combines the solar heating conductive film and the electrolytic cell process, and the solar heating conductive film and the electrolytic cell process are mutually promoted, so that the treatment effect can be effectively improved. The loaded CNT material can endow the film with conductivity while carrying out photo-thermal conversion, and the external electric field can obviously reduce the film pollution, improve the film flux and prolong the service life of the film.
Claims (7)
1. A method for removing antibiotic resistance genes based on solar heating film electrolysis is carried out by utilizing a solar heating film electrolysis system, wherein the solar heating film electrolysis system comprises a sewage container, a water pump and an electrolytic cell which are communicated; a water inlet and a water outlet are respectively arranged on two sides of the upper end of the electrolytic cell, and an anode and a cathode are fixed in the electrolytic cell between the water inlet and the water outlet; the anode and the cathode are respectively connected to the anode and the cathode of an external power supply through metal leads to form an electrolytic cell, and the bottom of the electrolytic cell is provided with a filtrate outlet;
the anode is a solar heating conductive film which is arranged on an annular supporting layer at the bottom of the electrolytic cell, and the cathode is a platinum electrode;
the solar heating conductive film is prepared by the following method:
(1) placing the PVDF membrane on dopamine hydrochloride solution, and standing for 10-20min to obtain an ultrafiltration membrane loaded with a polydopamine layer;
(2) dispersing the photo-thermal conductive material into a polyvinyl alcohol solution to obtain a photo-thermal conductive material-polyvinyl alcohol solution, and depositing or electrospinning the photo-thermal conductive material-polyvinyl alcohol solution onto the poly dopamine layer-loaded ultrafiltration membrane in the step (1) through pressure to form a PVA nanofiber network containing the photo-thermal conductive material, so as to obtain the solar heating conductive film; the photo-thermal conductive material is a carbon nano tube;
the method for removing the antibiotic resistance gene is as follows: the sewage containing the antibiotic resistance genes enters the electrolytic cell through the water inlet, the power supply is turned on, meanwhile, illumination is carried out, the solar heating conductive film absorbs solar energy to generate high temperature on the surface of the film, the antibiotic and resistant bacteria structures flowing to the surface of the film along with water are damaged, the resistance genes are released, the resistance genes are inactivated under the combined action of the high temperature and the acidic condition, and the sewage is filtered by the solar heating conductive film and then is discharged from a filtrate outlet to remove the antibiotic resistance genes.
2. The method for removing the antibiotic resistance gene based on the electrolysis of the solar heat-generating film according to claim 1, wherein in the step (1), the concentration of the dopamine hydrochloride solution is 1-5mg/mL, and the pH value is 8.5.
3. The method for removing antibiotic resistance genes based on solar heat generation film electrolysis according to claim 1, wherein in the step (2), when a pressure deposition mode is adopted, the mass ratio of the photothermal conductive material to the polyvinyl alcohol in the photothermal conductive material-polyvinyl alcohol solution is 1: 2 to 6, the pressure during pressure deposition is 0.1MPa, and the deposition time is 1 h.
4. The method for removing antibiotic resistance genes based on solar heat-generating film electrolysis according to claim 1, wherein in the step (2), when the electrospinning method is adopted, the concentration of the photothermal conductive material-the photothermal conductive material in the polyvinyl alcohol solution is 3 to 6wt%, the distance from the injector to the metal plate is 10cm, the injection rate of the injector is 0.5mL/min, the voltage is 10kV, and the spinning time is 3 hours.
5. The method for removing antibiotic resistance genes based on solar heat-generating film electrolysis according to claim 1, wherein the distance between the solar heat-generating conductive film and the platinum electrode is 3-6 cm.
6. The method for removing antibiotic resistance genes based on solar heat-generating film electrolysis according to claim 1, wherein the voltage of the power supply is 1-3V, and the illumination intensity is 1-3kw/m2。
7. The method for removing the antibiotic resistance gene based on the electrolysis of the solar heating film according to claim 1, wherein the sewage is secondary effluent of a sewage treatment plant, aquaculture wastewater, pharmaceutical wastewater or medical wastewater.
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