CN111362449A - 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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- CN111362449A CN111362449A CN202010101447.3A CN202010101447A CN111362449A CN 111362449 A CN111362449 A CN 111362449A CN 202010101447 A CN202010101447 A CN 202010101447A CN 111362449 A CN111362449 A CN 111362449A
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- persulfate
- sewage
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- antibiotic resistance
- resistance genes
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- 108090000623 proteins and genes Proteins 0.000 title claims abstract description 115
- JRKICGRDRMAZLK-UHFFFAOYSA-L peroxydisulfate Chemical compound [O-]S(=O)(=O)OOS([O-])(=O)=O JRKICGRDRMAZLK-UHFFFAOYSA-L 0.000 title claims abstract description 77
- PLKATZNSTYDYJW-UHFFFAOYSA-N azane silver Chemical compound N.[Ag] PLKATZNSTYDYJW-UHFFFAOYSA-N 0.000 title claims abstract description 45
- 238000000034 method Methods 0.000 title claims abstract description 33
- 230000003115 biocidal effect Effects 0.000 title claims abstract description 30
- NLXLAEXVIDQMFP-UHFFFAOYSA-N Ammonium chloride Substances [NH4+].[Cl-] NLXLAEXVIDQMFP-UHFFFAOYSA-N 0.000 title claims abstract description 18
- 230000003213 activating effect Effects 0.000 title claims abstract description 16
- 235000011114 ammonium hydroxide Nutrition 0.000 title claims description 13
- 239000010865 sewage Substances 0.000 claims abstract description 50
- 239000002244 precipitate Substances 0.000 claims abstract description 14
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims abstract description 12
- 229910001868 water Inorganic materials 0.000 claims abstract description 11
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 10
- 239000008139 complexing agent Substances 0.000 claims abstract description 7
- 239000013049 sediment Substances 0.000 claims abstract description 3
- 239000006228 supernatant Substances 0.000 claims abstract description 3
- LCPVQAHEFVXVKT-UHFFFAOYSA-N 2-(2,4-difluorophenoxy)pyridin-3-amine Chemical compound NC1=CC=CN=C1OC1=CC=C(F)C=C1F LCPVQAHEFVXVKT-UHFFFAOYSA-N 0.000 claims description 7
- CHQMHPLRPQMAMX-UHFFFAOYSA-L sodium persulfate Substances [Na+].[Na+].[O-]S(=O)(=O)OOS([O-])(=O)=O CHQMHPLRPQMAMX-UHFFFAOYSA-L 0.000 claims description 7
- 239000002351 wastewater Substances 0.000 claims description 6
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 claims description 4
- 238000005119 centrifugation Methods 0.000 claims description 4
- USHAGKDGDHPEEY-UHFFFAOYSA-L potassium persulfate Chemical compound [K+].[K+].[O-]S(=O)(=O)OOS([O-])(=O)=O USHAGKDGDHPEEY-UHFFFAOYSA-L 0.000 claims description 2
- 230000035484 reaction time Effects 0.000 claims description 2
- GGCZERPQGJTIQP-UHFFFAOYSA-N sodium;9,10-dioxoanthracene-2-sulfonic acid Chemical compound [Na+].C1=CC=C2C(=O)C3=CC(S(=O)(=O)O)=CC=C3C(=O)C2=C1 GGCZERPQGJTIQP-UHFFFAOYSA-N 0.000 claims 1
- 206010042618 Surgical procedure repeated Diseases 0.000 abstract 1
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- QJZYHAIUNVAGQP-UHFFFAOYSA-N 3-nitrobicyclo[2.2.1]hept-5-ene-2,3-dicarboxylic acid Chemical compound C1C2C=CC1C(C(=O)O)C2(C(O)=O)[N+]([O-])=O QJZYHAIUNVAGQP-UHFFFAOYSA-N 0.000 description 8
- 238000005516 engineering process Methods 0.000 description 8
- 239000004021 humic acid Substances 0.000 description 8
- 229910021607 Silver chloride Inorganic materials 0.000 description 7
- HKZLPVFGJNLROG-UHFFFAOYSA-M silver monochloride Chemical compound [Cl-].[Ag+] HKZLPVFGJNLROG-UHFFFAOYSA-M 0.000 description 7
- 108091003079 Bovine Serum Albumin Proteins 0.000 description 6
- 239000003242 anti bacterial agent Substances 0.000 description 6
- 229940088710 antibiotic agent Drugs 0.000 description 6
- 229940098773 bovine serum albumin Drugs 0.000 description 6
- 238000010586 diagram Methods 0.000 description 6
- 229910021642 ultra pure water Inorganic materials 0.000 description 6
- 239000012498 ultrapure water Substances 0.000 description 6
- 229910002651 NO3 Inorganic materials 0.000 description 5
- 238000011033 desalting Methods 0.000 description 5
- 230000007613 environmental effect Effects 0.000 description 5
- 230000008569 process Effects 0.000 description 5
- 238000003753 real-time PCR Methods 0.000 description 5
- AKHNMLFCWUSKQB-UHFFFAOYSA-L sodium thiosulfate Chemical compound [Na+].[Na+].[O-]S([O-])(=O)=S AKHNMLFCWUSKQB-UHFFFAOYSA-L 0.000 description 5
- 235000019345 sodium thiosulphate Nutrition 0.000 description 5
- 238000004659 sterilization and disinfection Methods 0.000 description 5
- 238000005660 chlorination reaction Methods 0.000 description 4
- 239000013612 plasmid Substances 0.000 description 4
- 238000011160 research Methods 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
- 239000002333 angiotensin II receptor antagonist Substances 0.000 description 3
- 229940125364 angiotensin receptor blocker Drugs 0.000 description 3
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- 244000144972 livestock Species 0.000 description 3
- 102000004169 proteins and genes Human genes 0.000 description 3
- 238000005070 sampling Methods 0.000 description 3
- 239000010802 sludge Substances 0.000 description 3
- 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
- 230000009471 action Effects 0.000 description 2
- 230000008901 benefit Effects 0.000 description 2
- 238000006555 catalytic reaction Methods 0.000 description 2
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- 229910001961 silver nitrate Inorganic materials 0.000 description 2
- 238000012546 transfer Methods 0.000 description 2
- 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
- 239000012028 Fenton's reagent Substances 0.000 description 1
- 108020005210 Integrons Proteins 0.000 description 1
- 239000004677 Nylon Substances 0.000 description 1
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 description 1
- 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
- 230000001174 ascending effect Effects 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
- 230000006872 improvement Effects 0.000 description 1
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- 238000007146 photocatalysis Methods 0.000 description 1
- 230000001699 photocatalysis Effects 0.000 description 1
- 230000000704 physical effect Effects 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
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- 230000001737 promoting effect Effects 0.000 description 1
- 150000003254 radicals Chemical class 0.000 description 1
- 239000003642 reactive oxygen metabolite Substances 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
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- 238000011069 regeneration method Methods 0.000 description 1
- 230000000452 restraining effect Effects 0.000 description 1
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- -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
- 230000007480 spreading Effects 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
- 229960002180 tetracycline Drugs 0.000 description 1
- 229930101283 tetracycline Natural products 0.000 description 1
- 235000019364 tetracycline Nutrition 0.000 description 1
- 150000003522 tetracyclines Chemical class 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
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- Life Sciences & Earth Sciences (AREA)
- Hydrology & Water Resources (AREA)
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Purification Treatments By Anaerobic Or Anaerobic And Aerobic Bacteria Or Animals (AREA)
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 a complexing agent into the sewage to ensure that the precipitate is just completely dissolved; 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 have certain effect on the removal of the resistance genes, can respectively reduce the resistance genes inside and outside cells by 4 orders of magnitude under the conditions that the pH is 7 and the exposure of chlorine is 50 (mg × min)/L-80 (mg × min)/L, and has the 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. The disinfection technology represented by chlorination and ultraviolet has wide applicationGeneral, mature method, low equipment failure rate and low operation cost, but each of them has some short plates, such as the disadvantages of chlorination including selectivity for removing the resistance gene, the need of adding a larger amount of chlorine (Journal of Environmental sciences 2014.26(6). 1238) -1242) for achieving effective removal of the resistance gene, and the possibility of changing the cell membrane permeability and further promoting the propagation and diffusion of the resistance gene (Environmental science 1242)&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).8666-8673), Fenton's reagent (Environmental Science and pollution Research, 2015.22(9).7037-7044) and the like. 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 resistance to the environmentRisk of sexual genes. In addition, a literature (Waterreach.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+To makeAg 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 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. 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 D was sequentially addedNA, 0.2mM Ag+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+Activation system (30 min degradation rate is only 3.6 orders of magnitude when PS is 20mM)) The improvement is obvious.
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 Ca is used as a main ion influencing the hardness of the water body2+，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 orders of magnitude after 30min of the reaction.
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 effect of different kinds of sewage on the degradation resistance gene effect of the silver ammonia/persulfate system is shown in FIG. 8, and the effect on the degradation resistance gene effect of the silver ammonia/persulfate system can be found in experiments with ultrapure waterCompared with the prior art, various sewage has certain inhibition effect on degradation and is accompanied by 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 be reduced by 0.28 orders of magnitude in 10min, and when the concentration of PS is increased to 5mM, the concentration can be reduced by 1.6-2.3 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 (9)
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, sewage is treatedAdding Ag into water+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.
2. The method for removing antibiotic resistance genes by activating persulfate through silver-ammonia solution as claimed in claim 1, wherein the Ag in the first step+Derived from a soluble silver salt.
3. The method for removing antibiotic resistance genes by using the silver ammonia solution to activate persulfate as claimed in claim 1 or 2, wherein the step of adding Ag into the sewage is+Make Ag in sewage+The concentration is 0.2 mM-200 mM.
4. The method for removing the antibiotic resistance gene by activating the persulfate through the silver-ammonia solution as recited in claim 1, wherein the complexing agent in the second step is ammonia water.
5. The method for removing antibiotic resistance genes by activating persulfate through silver ammonia solution according to claim 1, wherein the persulfate in the third step is sodium persulfate and/or potassium persulfate.
6. The method for removing antibiotic resistance genes by using the silver ammonia solution to activate the persulfate according to the claim 1 or 5, wherein the concentration of the persulfate in the wastewater in the third step is 0.5mM to 200 mM.
7. 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.
8. The method for removing antibiotic resistance genes by using the silver-ammonia solution to activate persulfate according to claim 1, wherein concentrated hydrochloric acid is added in the fourth step so that the pH value is less than or equal to 6 and less than or equal to 9.
9. 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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| CN101172692A (en) * | 2007-09-28 | 2008-05-07 | 大连海事大学 | Method for processing red tide with sulphuric acid free radical |
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| US20180036254A1 (en) * | 2012-03-16 | 2018-02-08 | The Regents Of The University Of California | NOVEL RNAi MOLECULE DELIVERY PLATFORM BASED ON SINGLE-siRNA AND shRNA NANOCAPSULES |
| CN110526381A (en) * | 2019-09-20 | 2019-12-03 | 中国科学院城市环境研究所 | Co-MOFs base macroscopic view composite material generates the method that active oxygen species remove emerging pollutant |
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| US20080107707A1 (en) * | 2006-07-06 | 2008-05-08 | Regents Of The University Of Colorado | Polymerizable antimicrobial composition |
| CN101172692A (en) * | 2007-09-28 | 2008-05-07 | 大连海事大学 | Method for processing red tide with sulphuric acid free radical |
| CN102883783A (en) * | 2010-04-26 | 2013-01-16 | 三菱瓦斯化学株式会社 | Treatment agent for decomposition of chemical substance which comprises persulfuric acid salt and silver complex, and method for decomposition of chemical substance using same |
| US20180036254A1 (en) * | 2012-03-16 | 2018-02-08 | The Regents Of The University Of California | NOVEL RNAi MOLECULE DELIVERY PLATFORM BASED ON SINGLE-siRNA AND shRNA NANOCAPSULES |
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| CN110526381A (en) * | 2019-09-20 | 2019-12-03 | 中国科学院城市环境研究所 | Co-MOFs base macroscopic view composite material generates the method that active oxygen species remove emerging pollutant |
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