CN111362449B - Method for removing antibiotic resistance genes by activating persulfate through silver ammonia solution - Google Patents
Method for removing antibiotic resistance genes by activating persulfate through silver ammonia solution Download PDFInfo
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- CN111362449B CN111362449B CN202010101447.3A CN202010101447A CN111362449B CN 111362449 B CN111362449 B CN 111362449B CN 202010101447 A CN202010101447 A CN 202010101447A CN 111362449 B CN111362449 B CN 111362449B
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- 108090000623 proteins and genes Proteins 0.000 title claims abstract description 109
- JRKICGRDRMAZLK-UHFFFAOYSA-L peroxydisulfate Chemical compound [O-]S(=O)(=O)OOS([O-])(=O)=O JRKICGRDRMAZLK-UHFFFAOYSA-L 0.000 title claims abstract description 72
- PLKATZNSTYDYJW-UHFFFAOYSA-N azane silver Chemical compound N.[Ag] PLKATZNSTYDYJW-UHFFFAOYSA-N 0.000 title claims abstract description 39
- 238000000034 method Methods 0.000 title claims abstract description 28
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- NLXLAEXVIDQMFP-UHFFFAOYSA-N Ammonium chloride Substances [NH4+].[Cl-] NLXLAEXVIDQMFP-UHFFFAOYSA-N 0.000 title claims abstract description 13
- 230000003213 activating effect Effects 0.000 title claims abstract description 13
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- LCPVQAHEFVXVKT-UHFFFAOYSA-N 2-(2,4-difluorophenoxy)pyridin-3-amine Chemical group NC1=CC=CN=C1OC1=CC=C(F)C=C1F LCPVQAHEFVXVKT-UHFFFAOYSA-N 0.000 claims description 6
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- 239000004021 humic acid Substances 0.000 description 8
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- 108091003079 Bovine Serum Albumin Proteins 0.000 description 6
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- 239000013612 plasmid Substances 0.000 description 4
- SQGYOTSLMSWVJD-UHFFFAOYSA-N silver(1+) nitrate Chemical compound [Ag+].[O-]N(=O)=O SQGYOTSLMSWVJD-UHFFFAOYSA-N 0.000 description 4
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 3
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- 241000894006 Bacteria Species 0.000 description 2
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 2
- 102000053602 DNA Human genes 0.000 description 2
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- RBWNDBNSJFCLBZ-UHFFFAOYSA-N 7-methyl-5,6,7,8-tetrahydro-3h-[1]benzothiolo[2,3-d]pyrimidine-4-thione Chemical compound N1=CNC(=S)C2=C1SC1=C2CCC(C)C1 RBWNDBNSJFCLBZ-UHFFFAOYSA-N 0.000 description 1
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- 239000004098 Tetracycline Substances 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 239000012190 activator Substances 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
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- 229910001385 heavy metal Inorganic materials 0.000 description 1
- MGZTXXNFBIUONY-UHFFFAOYSA-N hydrogen peroxide;iron(2+);sulfuric acid Chemical compound [Fe+2].OO.OS(O)(=O)=O MGZTXXNFBIUONY-UHFFFAOYSA-N 0.000 description 1
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- 230000000452 restraining effect Effects 0.000 description 1
- -1 silver ammonia activated PS Chemical class 0.000 description 1
- 229940096017 silver fluoride Drugs 0.000 description 1
- REYHXKZHIMGNSE-UHFFFAOYSA-M silver monofluoride Chemical compound [F-].[Ag+] REYHXKZHIMGNSE-UHFFFAOYSA-M 0.000 description 1
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- 235000019364 tetracycline Nutrition 0.000 description 1
- 150000003522 tetracyclines Chemical class 0.000 description 1
- ZNRSXPDDVNZGEN-UHFFFAOYSA-K trisodium;chloride;sulfate Chemical compound [Na+].[Na+].[Na+].[Cl-].[O-]S([O-])(=O)=O ZNRSXPDDVNZGEN-UHFFFAOYSA-K 0.000 description 1
- 238000009281 ultraviolet germicidal irradiation Methods 0.000 description 1
Images
Classifications
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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
- C02F9/00—Multistage treatment of water, waste water or sewage
-
- 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
- C02F1/38—Treatment of water, waste water, or sewage by centrifugal separation
-
- 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
- C02F1/44—Treatment of water, waste water, or sewage by dialysis, osmosis or reverse osmosis
-
- 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
- C02F1/52—Treatment of water, waste water, or sewage by flocculation or precipitation of suspended impurities
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/66—Treatment of water, waste water, or sewage by neutralisation; pH adjustment
Abstract
The invention provides a method for removing antibiotic resistance genes by activating persulfate through a silver-ammonia solution, which comprises the following steps: adding Ag into sewage+Generating a precipitate; adding complexing agent into the sewage to make precipitationCompletely dissolving; adding persulfate into the sewage, and reacting for a certain time to fully degrade antibiotic resistance genes; adding concentrated hydrochloric acid into the sewage to ensure that the pH is less than or equal to 9 and Ag+Re-precipitating; centrifuging the sewage, and separating supernatant from precipitate; the sediment was resuspended in contaminated water and the procedure repeated. The method for removing the antibiotic resistance gene by activating persulfate through the silver-ammonia extraction solution can efficiently remove the resistance gene and can realize the removal of Ag+Can be repeatedly used.
Description
Technical Field
The invention relates to an environmental pollution control technology, in particular to a method for removing antibiotic resistance genes by activating persulfate through a silver-ammonia solution.
Background
Due to the non-standard use of antibiotics in the industries of human medicine, livestock breeding and the like, a large amount of antibiotics which are not digested and absorbed enter the environment and become the selective pressure of the environment, so that microorganisms are forced to evolve to generate Antibiotic Resistance Genes (ARG) and express antibiotic resistance. Antibiotic resistance genes can also be transmitted and spread in the environment by means of Horizontal Gene Transfer (HGT) and the like. The widespread development and spread of antibiotic resistance can make some diseases that are currently curable with antibiotics difficult to cure or even life-threatening. Thus, further development of antibiotic resistance is being stopped. Among them, reducing the content of antibiotics in the environment, removing resistant bacteria (ARB) in the environment, and controlling the spread and spread of resistance genes are three major factors controlling the progress of antibiotic resistance.
Particularly, resistance genes have been considered as a novel environmental pollutant and have been paid much attention in recent years because of their replicability, reproducibility and transmissibility. As the antibiotics and the resistance genes can be discharged into a sewage treatment field along with the livestock and poultry breeding sewage, the pharmaceutical sewage, the medical sewage and the domestic sewage for centralized treatment, and the heavy metal ions have the enhancement effect on the selective pressure of the resistance genes, the ARBs and the resistance genes are enriched in the sewage treatment plant. At the same time, the ARBs and the resistance genes reenter the natural environment through the ways of sludge utilization, sewage discharge and the like. Sewage plants are therefore an important source and sink for ARBs and resistance genes. Therefore, how to find a quick and effective method for effectively removing antibiotic resistance genes in sewage is an important problem for restraining the development of antibiotic resistance at present.
The existing technologies for removing resistance genes mainly comprise disinfection technologies represented by chlorination and ultraviolet, constructed wetlands, coagulation and microfiltration and the like. For example, chlorination, UV, UV/H are evaluated in the literature (Water research.2017.123.783-793)2O2The system has certain effect on the removal of the resistance genes, and the three processes can reduce the resistance genes inside and outside the cells by 4 orders of magnitude under the conditions that the chlorine exposure is 50 (mg × min)/L-80 (mg × min)/L under the condition that the pH is 7. At an ultraviolet intensity of 40mJ/cm2(typical UV intensity used for disinfection), UV can reduce the extracellular and intracellular resistance genes by 1.8-2.6 and 1.1-1.6 orders of magnitude. UV/H2O2The degradation effect of the system on intracellular resistance genes is approximately equivalent to that of the UV system, but the degradation rate of the extracellular resistance genes is 1.5 times that of the intracellular resistance genes. Although the disinfection technologies represented by chlorination and ultraviolet have the advantages of wide application, mature method, low equipment failure rate and running cost, etc., the disinfection technologies have some short plates, such as chlorination, which have the disadvantages of selectivity for removing the resistance gene, addition of a large amount of chlorine (Journal of Environmental sciences 2014.26(6). 1238) -1242) for realizing effective removal of the resistance gene, and change of cell membrane permeability to promote the propagation and diffusion of the resistance gene (Environmental science)&technology.2015.49(9). 5771-. Although UV disinfection does not produce disinfection by-products, the damage to the resistance gene is limited, and thus there is a problem that the content of the resistance gene increases again. In addition to this, UV-irradiation also has selectivity for the removal of resistance genes (Environmental science)&technology.2015.49(9). 5771-. In addition to the above methods, there have been reports of using ozone catalytic oxidation (Chemosphere,2016,150: 702-), photocatalysis (Environmental science)&technology, 2018.52(15), 8666 and 8673), Fenton's reagent (Environmental Science and pollution)n Research, 2015.22(9).7037-7044), etc. Although the method has good removal effect on resistance genes, the method also has the defects of incomplete removal, easy regeneration of the resistance genes, long action time (Catalysis today.2015.240.55-60), easy change of cell membrane permeability to promote resistance propagation (Catalysis today.2015.240.55-60), high cost and the like. In recent years, constructed wetlands have been tried to treat contamination with resistance genes. The artificial wetland is mainly characterized in that a ground ecosystem is formed by a substrate, microorganisms and plants, and pollutants are removed through physical action, chemical action and biological action. The document (Chemical Engineering journal.2017.308.692-699) researches the effect of the drooping direct current artificial wetland in the two flowing modes of the sewage ascending and descending on removing the integron int I and the tetracycline resistance gene of the mobile element, and the result shows that the removal rate can reach 33% -99%, thereby showing that the artificial wetland system has certain resistance gene removal effect. But at the same time, the relative concentration of the resistance genes in the water is improved, which means that the sewage treated by the artificial wetland has higher risk of the resistance genes for the environment. In addition, a literature (Water research.2019.159.145-152.) reports that the coagulation and microfiltration coupling process can effectively remove extracellular resistance genes, and the removal efficiency can reach more than 5 orders of magnitude. However, the technology only transfers the resistance gene into the excess sludge without degrading the resistance gene, and if the sludge is not properly treated, the risk of spreading the resistance gene still exists.
Therefore, there is a need to develop novel processes capable of efficiently removing the resistance gene.
Disclosure of Invention
The invention aims to provide a method for removing antibiotic resistance genes by activating persulfate through a silver ammonia solution aiming at the problem that the resistance genes are difficult to remove at present, the method can be used for efficiently removing the resistance genes and can realize the purpose that Ag can be removed+Can be repeatedly used.
In order to achieve the purpose, the invention adopts the technical scheme that: a method for removing antibiotic resistance genes by activating persulfate through a silver ammonia solution comprises the following steps:
step one, adding Ag into sewage+Generating a precipitate;
step two, adding a complexing agent into the sewage to ensure that the precipitate is just completely dissolved;
thirdly, adding persulfate into the sewage, and reacting for a certain time to fully degrade antibiotic resistance genes;
step four, adding concentrated hydrochloric acid into the sewage to ensure that the pH is less than or equal to 9 and Ag is+Re-precipitating;
step five, centrifuging the sewage, and separating supernatant from precipitate;
and step six, suspending the sediment again by using sewage, and repeating the step two, the step three, the step four and the step five.
Further, the sewage is sewage containing antibiotics.
Further, step one of Ag+From soluble silver salts, such as silver nitrate, silver fluoride, silver perchlorate, preferably silver nitrate.
Further, the step of adding Ag to the wastewater+Make Ag in sewage+The concentration is 0.2 mM-200 mM, preferably 0.2-2 mM.
Further, the complexing agent in the second step is a complexing agent capable of dissolving silver chloride precipitate, and preferably ammonia water. Step two the complexing agent is added so that the precipitate is completely dissolved.
Further, in the third step, the persulfate is sodium persulfate and/or potassium persulfate.
Further, the concentration of the persulfate in the wastewater obtained in the third step is 0.5 mM-200 mM, preferably 0.5 mM-20 mM.
Further, the reaction time in the third step is more than 10min, preferably 10min to 30 min.
And further, adding concentrated hydrochloric acid in the fourth step to ensure that the pH value is more than or equal to 6 and less than or equal to 9.
Further, the centrifugation in the step five is used for completely separating the solution and the silver chloride precipitate, the rotating speed is preferably 11000rpm or more, and the centrifugation time is preferably 5min or more.
The principle of the process for effectively removing the resistance genes provided by the invention is as follows:
Ag+complexing with aqueous ammonia to form Ag (NH)3)2 +By Ag (NH)3)2 +Strong interaction with DNA, making Ag (NH)3)2 +Inserted into the DNA molecule, and after persulfate is added, free Ag (NH) on the one hand3)2 +Can activate persulfate to generate singlet oxygen, and on the other hand, Ag (NH) inserted between double chains in the DNA molecule3)2 +It is also possible to activate persulfate salts to generate singlet oxygen, and thus singlet oxygen destroys DNA simultaneously from the inside and outside of the DNA molecule, resulting in degradation of DNA. Ag (NH) after DNA destruction3)2 +Is released by adding sufficient hydrochloric acid to shift the precipitation dissolution equilibrium of silver chloride toward silver chloride formation, thereby allowing Ag+Is precipitated in large amounts. After the precipitate is centrifugally collected, reducing silver chloride and adding the silver chloride into the sewage containing the resistance gene again, and adding a proper amount of ammonia water to ensure that the precipitate of the silver chloride is dissolved and balanced to generate Ag (NH)3)2 +Moving in the direction to further realize Ag+Can be repeatedly used.
Compared with the prior art, the method for removing the antibiotic resistance gene by activating the persulfate through the silver-ammonia solution has the following advantages: the method has the advantages of good resistance gene removal effect, high reaction rate, strong anti-interference capability, low consumption of persulfate, complete removal of the resistance gene, no content re-rise, effective killing of resistant bacteria while removing the resistance gene, and Ag activator+Can be repeatedly used, and the consumption of the persulfate is less, so the cost is lower.
Therefore, the invention provides a resistance gene removal method with stronger anti-interference capability and better removal effect, and has certain feasibility in the actual sewage treatment process. The methods developed herein are of great interest for controlling the production, transmission and spread of resistance genes in an environment. In addition, the invention helps to promote the Ag-based+The application of the activated free radical generation reaction in the real sewage treatment process.
Drawings
FIG. 1 shows different Ag+The effect of the concentration on the degradation resistance gene effect of the silver ammonia/persulfate system is shown schematically;
FIG. 2 shows different NH groups3The effect of the concentration on the degradation resistance gene effect of the silver ammonia/persulfate system is shown schematically;
FIG. 3 is a schematic diagram showing the effect of different persulfate concentrations on the degradation resistance gene effect of a silver ammonia/persulfate system;
FIG. 4 is a schematic diagram showing the effect of common components in real sewage on the degradation resistance gene effect of a silver ammonia/persulfate system, specifically, the effect of metal ions on the degradation resistance gene effect of the silver ammonia/persulfate system;
FIG. 5 is a schematic diagram showing the influence of common components in real sewage on the degradation resistance gene effect of a silver ammonia/persulfate system, specifically, the influence of anions on the degradation resistance gene effect of the silver ammonia/persulfate system;
FIG. 6 is a schematic diagram showing the influence of common components in real sewage on the degradation resistance gene effect of a silver ammonia/persulfate system, specifically, the influence of humic acid on the degradation resistance gene effect of the silver ammonia/persulfate system;
FIG. 7 is a schematic diagram showing the influence of common components in real sewage on the degradation resistance gene effect of a silver ammonia/persulfate system, specifically, the influence of protein on the degradation resistance gene effect of the silver ammonia/persulfate system;
FIG. 8 is a schematic diagram showing the effect of different types of wastewater on the effect of the degradation resistance genes of a silver ammonia/persulfate system;
FIG. 9 shows the steps of the method for removing antibiotic resistance genes by using silver ammonia solution to activate persulfate.
Detailed Description
The invention is further illustrated by the following examples:
example 1
Different Ag+Influence of concentration on effect of silver ammonia/persulfate system on degradation resistance gene
To the wells of a 96-well plate, 10mg/L of pUC 57 plasmid DNA, 2. mu.M, 20. mu.M, 0.2mM, 2mM of Ag were added in this order+70mM NH30.5mM of sodium chlorideSodium sulfate, each well diluted to 100. mu.L with ultrapure water, shaken at 150rpm for 30min, quenched by adding 4.5. mu.L of sodium thiosulfate solution (1mol/L) at 1min, 2min, 5min, 10min, 20min, and 30min, respectively, and sampled at 50. mu.L, after desalting treatment, the DNA content in the sample was determined using fluorescent quantitative PCR. Method for removing antibiotic resistance genes by activating persulfate with silver-ammonia solution as shown in FIG. 9, different Ag materials+The effect of concentration on the effect of the degradation resistance gene of the silver ammonia/persulfate system is shown in figure 1: when Ag is present+At a lower concentration of 20. mu.M, 0.5mM PS had little effect on the degradation of the resistance gene, when Ag was added+When the concentration is increased to 0.2mM and 2mM, the concentration of the resistance gene can be respectively reduced by 2.5 and 4.5 orders of magnitude in 30min, thereby indicating that the Ag+The content has a large influence on the effect of activating PS.
Example 2
Different NH3Influence of concentration on effect of silver ammonia/persulfate system on degradation resistance gene
To the wells of a 96-well plate, 10mg/L of pUC 57 plasmid DNA, 0.2mM of Ag were added in this order+70mM, 35mM, 7mM, 0.7mM NH30.5mM sodium persulfate, each well diluted to 100. mu.L with ultrapure water, shaking at 150rpm for 30min, adding 4.5. mu.L of sodium thiosulfate solution (1mol/L) at 1min, 2min, 5min, 10min, 20min, 30min to terminate the reaction, sampling 50. mu.L, desalting, and determining the DNA content in the sample by using fluorescence quantitative PCR. Different NH3Effect of concentration on the Effect of degradation resistance Gene of silver Ammonia/persulfate System As shown in FIG. 2, it can be found that in ultrapure Water system, NH is accompanied by NH3·H2The increasing of the O concentration and the gradually increasing of the degradation effect are carried out in NH3·H2At an O concentration of 0.7mM, the reaction was carried out for 30min with almost no degradation of the resistance gene but with NH3·H2The concentration of O is increased to 7mM, and the concentration of the resistance gene can be reduced by 2.6 orders of magnitude after 30min, and NH is continuously increased3·H2O concentrations to 35mM and 70mM, the resistance gene concentration will drop by 4.5 and 4.7 orders of magnitude at 30 min.
Example 3
Effect of different Persulfate (PS) concentrations on the Effect of degrading resistant genes in silver Ammonia/persulfate systems
To the wells of a 96-well plate, 10mg/L of pUC 57 plasmid DNA, 0.2mM of Ag were added in this order+70mM NH310mM, 5mM, 0.5mM, 1mM sodium persulfate, each well diluted to 100. mu.L with ultrapure water, shaking at 150rpm for 30min, terminating the reaction by adding 4.5. mu.L of sodium thiosulfate solution (1mol/L) at 1min, 2min, 4min, 6min, 8min, 10min, respectively, and sampling 50. mu.L, after desalting treatment, the DNA content in the sample was determined using fluorescent quantitative PCR. The effect of different persulfate concentrations on the degradation of the resistance gene of the silver ammonia/persulfate system is shown in figure 3, when the PS concentration is 0.5mM, the degradation rate is gradually increased within 30min, the resistance gene concentration can be reduced by 3.5 orders of magnitude after the reaction is carried out for 30min, and the degradation effect is further increased when the PS concentration is continuously increased, when the PS concentrations are 5mM and 10mM, the degradation effect can reach 4.5 orders of magnitude and 4.7 orders of magnitude within 2min, and compared with the Ag, the degradation effect can reach 4.5 orders of magnitude and 4.7 orders of magnitude within 2min+The activation system (the degradation rate is only 3.6 orders of magnitude at 30min when the PS is 20mM) is obviously improved.
Example 4
Influence of common components in real sewage on degradation resistance gene effect of silver ammonia/persulfate system
To the wells of a 96-well plate, pUC 57 plasmid DNA (10mg/L), Ag was added+(0.2mM)， NH3(70mM), metal ion (K) is added to the system+，Ca2+，Mg2+(ii) a Final concentrations 0.2mM and 20mM), anion (SO)4 2-，NO3 -，Cl-(ii) a Final concentrations of 2mM and 200mM), Humic Acid (HA) and Bovine Serum Albumin (BSA), concentrations of 5, 10, 15, 20 mg/L. Finally, 0.5mM sodium persulfate is added to start the reaction, the reaction is shaken at 150rpm for 30min, 4.5 mu L of sodium thiosulfate solution (1mol/L) is added at 1min, 2min, 5min, 10min, 20min and 30min to stop the reaction, 50 mu L of the solution is sampled, and after desalting treatment, the DNA content in the sample is determined by using fluorescence quantitative PCR. The influence of common components in real sewage on the effect of the degradation resistance gene of the silver ammonia/persulfate system is shown in figures 4-7, and the influence is taken as the influence on the water hardnessMain ion of (2), Ca2+，Mg2+Ions are common in water bodies. Ca can be found as shown in FIG. 42+Has very obvious inhibiting effect on degradation, Ca2+When the concentration is 0.2mM, the concentration is reduced by 0.9 orders of magnitude only in 30min, and when Ca is added2+The degradation effect at 30min was only 0.2 orders of magnitude when the concentration was further increased to 20 mM. And Mg2+Then relative to Ca2+The effect on degradation is small, although when Mg is used2+The 30min resistance gene only degrades by 0.6 orders of magnitude at 20mM, but when Mg2+When the concentration is reduced to 0.2mM, the degradation is hardly affected. And K+The effect on the silver ammonia/PS system is smaller, and the 30min can be reduced to more than 3 orders of magnitude no matter the concentration is 20mM or 0.2 mM. Alternatively, SO as shown in FIG. 54 2-，NO3 -With Cl-The influence on the degradation effect of the silver ammonia/PS system is approximately the same, and SO is added4 2-，NO3 -With Cl-Has inhibition on degradation and high concentration of SO4 2-，NO3 -With Cl-Degradation of the resistance gene was almost completely inhibited, while 2mM SO4 2-With NO3 -The influence on the system is small, and the degradation effect can still reach 2.8 to 3.2 orders of magnitude in 30 min. Due to the ubiquitous existence of soluble organic pollutants in sewage systems, humic acid and protein (bovine serum albumin (BSA) is taken as a representative) are selected as research objects, and the influence of the humic acid and the protein on degradation resistance genes of the silver ammonia/PS system is examined. As shown in FIGS. 4-6, when the HA concentration is lower than 5 and 10mg/L, the degradation efficiency is slightly inhibited, and the resistance gene concentration can be reduced by 3-3.3 orders of magnitude in 30 min. However, when the HA concentration is increased to 15 and 20mg/L, the degradation is remarkably inhibited, and finally, the resistance gene can be reduced by 0.6-1.0 orders of magnitude. While HA itself, as a contaminant, may compete with DNA for reactive oxygen species generated by silver ammonia activated PS to inhibit degradation of the resistance gene. However, as shown in FIGS. 4 to 7, the effect of BSA on the degradation of the resistance gene is small, and although the degradation efficiency is slightly decreased as the BSA concentration is increased, the concentration of the resistance gene can be decreased by 3.4 to 3.9 after 30min of the reactionAn order of magnitude.
Example 5
Influence of different kinds of sewage on degradation resistance gene effect of silver ammonia/persulfate system
The 4 kinds of water selected in the experiment are respectively ultrapure water, secondary effluent of a campus sewage treatment plant in the Panjin school district of the university of major graduates, river water of a small river in the campus of the Panjin school district of the university of major graduates and influent water of a sewage treatment station of a permanent culture farm in the city of Nanchang. After the water sample was withdrawn, the sample was preliminarily filtered through a 200-mesh nylon filter and a 0.45 μm filter in this order. Then, DNA (10mg/L) and Ag were added to the 96-well plate in order+(0.2mM)， NH3(35 or 70mM), adding a corresponding kind of waste water to make the volume 100. mu.L, then adding sodium persulfate (0.5 or 5mM) to start the reaction, shaking at 150rpm for 30min, adding 4.5. mu.L of a sodium thiosulfate solution (1mol/L) to stop the reaction 30min later, and taking 50. mu.L of the sample, after desalting treatment, determining the DNA content in the sample by using fluorescence quantitative PCR. The influence of different types of sewage on the degradation resistance gene effect of the silver ammonia/persulfate system is shown in FIG. 8, and experiments show that compared with ultrapure water, various types of sewage have certain inhibition effect on degradation, and in addition, with NH3·H2The degradation effect is improved to a certain extent by increasing the concentration of O or PS. After reacting for 30min in an ultrapure water system, the resistance gene with high PS concentration (5mM) can be reduced by 3-4 orders of magnitude, and the resistance gene with low PS concentration (0.5mM) can also be reduced by nearly 3 orders of magnitude. However, in the campus river or other two sewage systems, the degradation of resistance gene is significantly inhibited under the condition of low PS concentration or low ammonia concentration, for example, in the campus river system, no matter NH when PS is 0.5mM3·H2The resistance gene is reduced by 0.2-0.3 orders of magnitude for O, and NH is increased when PS is 5mM3·H2The degradation efficiency was slightly increased to 0.56 orders of magnitude at an O concentration of 35mM, whereas NH was slightly increased3·H2The increase of O to 70mM and 30min can reduce the resistance gene by 2.47 orders of magnitude. The secondary effluent of the campus sewage plant is more sensitive to the PS concentration, and no matter NH, when the PS concentration is 0.5mM3·H2The concentration of O can only reduce the resistance gene by 0.28 orders of magnitude in 10minWhen the PS concentration is increased to 5mM, the PS concentration can be reduced by 1.6 to 2.3 orders of magnitude in 10 min. The livestock and poultry breeding wastewater has the most obvious effect of inhibiting the degradation effect on the whole, namely NH3·H2The reduction in the resistance gene was only 1 order of magnitude with 70mM O and 5mM PS.
Finally, it should be noted that: the above embodiments are only used to illustrate the technical solution of the present invention, and not to limit the same; while the invention has been described in detail and with reference to the foregoing embodiments, it will be understood by those skilled in the art that: the technical solutions described in the foregoing embodiments may still be modified, or some or all of the technical features may be equivalently replaced; and the modifications or the substitutions do not make the essence of the corresponding technical solutions depart from the scope of the technical solutions of the embodiments of the present invention.
Claims (4)
1. A method for removing antibiotic resistance genes by activating persulfate through a silver ammonia solution is characterized by comprising the following steps:
step one, adding Ag into sewage+Make Ag in sewage+The concentration is 0.2 mM-200 mM; generating a precipitate; the Ag is+From soluble silver salts;
step two, adding a complexing agent into the sewage to ensure that the precipitate is just completely dissolved; the complexing agent is ammonia water;
thirdly, adding persulfate into the sewage, and reacting for a certain time to fully degrade antibiotic resistance genes; the persulfate is sodium persulfate and/or potassium persulfate;
step four, adding concentrated hydrochloric acid into the sewage to ensure that the pH is more than or equal to 6 and less than or equal to 9 and Ag+Re-precipitating;
step five, centrifuging the sewage, and separating supernatant from precipitate;
and step six, suspending the sediment again by using sewage, and repeating the step two, the step three, the step four and the step five.
2. The method for removing antibiotic resistance genes by using the silver-ammonia solution to activate persulfate according to claim 1, wherein the concentration of the persulfate in the wastewater in the third step is 0.5 mM-200 mM.
3. The method for removing antibiotic resistance genes by activating persulfate through silver-ammonia solution as claimed in claim 1, wherein the reaction time in the third step is more than 10 min.
4. The method for removing the antibiotic resistance genes by activating the persulfate through the silver-ammonia solution as claimed in claim 1, wherein the centrifugation rotation speed in the step five is more than 11000rpm, and the centrifugation time is more than 5 min.
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