CN113896276A - Method for removing antibiotics and resistance genes in sewage by using ultraviolet/peroxyacetic acid - Google Patents
Method for removing antibiotics and resistance genes in sewage by using ultraviolet/peroxyacetic acid Download PDFInfo
- Publication number
- CN113896276A CN113896276A CN202111152435.4A CN202111152435A CN113896276A CN 113896276 A CN113896276 A CN 113896276A CN 202111152435 A CN202111152435 A CN 202111152435A CN 113896276 A CN113896276 A CN 113896276A
- Authority
- CN
- China
- Prior art keywords
- sewage
- ultraviolet
- antibiotics
- resistance genes
- peroxyacetic acid
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
- 239000010865 sewage Substances 0.000 title claims abstract description 117
- KFSLWBXXFJQRDL-UHFFFAOYSA-N Peracetic acid Chemical compound CC(=O)OO KFSLWBXXFJQRDL-UHFFFAOYSA-N 0.000 title claims abstract description 85
- 108090000623 proteins and genes Proteins 0.000 title claims abstract description 38
- 239000003242 anti bacterial agent Substances 0.000 title claims abstract description 36
- 229940088710 antibiotic agent Drugs 0.000 title claims abstract description 36
- 238000000034 method Methods 0.000 title claims abstract description 32
- 239000007788 liquid Substances 0.000 claims description 14
- 239000002351 wastewater Substances 0.000 claims description 5
- 238000003756 stirring Methods 0.000 claims description 2
- 238000004065 wastewater treatment Methods 0.000 claims description 2
- 238000004659 sterilization and disinfection Methods 0.000 abstract description 26
- 238000006243 chemical reaction Methods 0.000 abstract description 8
- 230000008569 process Effects 0.000 abstract description 7
- 230000005855 radiation Effects 0.000 abstract description 4
- 230000035484 reaction time Effects 0.000 abstract description 2
- 239000000203 mixture Substances 0.000 abstract 1
- 230000000052 comparative effect Effects 0.000 description 23
- 230000000694 effects Effects 0.000 description 18
- 239000006227 byproduct Substances 0.000 description 8
- 239000003120 macrolide antibiotic agent Substances 0.000 description 8
- ULGZDMOVFRHVEP-RWJQBGPGSA-N Erythromycin Chemical compound O([C@@H]1[C@@H](C)C(=O)O[C@@H]([C@@]([C@H](O)[C@@H](C)C(=O)[C@H](C)C[C@@](C)(O)[C@H](O[C@H]2[C@@H]([C@H](C[C@@H](C)O2)N(C)C)O)[C@H]1C)(C)O)CC)[C@H]1C[C@@](C)(OC)[C@@H](O)[C@H](C)O1 ULGZDMOVFRHVEP-RWJQBGPGSA-N 0.000 description 6
- JGSARLDLIJGVTE-MBNYWOFBSA-N Penicillin G Chemical compound N([C@H]1[C@H]2SC([C@@H](N2C1=O)C(O)=O)(C)C)C(=O)CC1=CC=CC=C1 JGSARLDLIJGVTE-MBNYWOFBSA-N 0.000 description 6
- 239000004098 Tetracycline Substances 0.000 description 6
- MYSWGUAQZAJSOK-UHFFFAOYSA-N ciprofloxacin Chemical compound C12=CC(N3CCNCC3)=C(F)C=C2C(=O)C(C(=O)O)=CN1C1CC1 MYSWGUAQZAJSOK-UHFFFAOYSA-N 0.000 description 6
- 239000003344 environmental pollutant Substances 0.000 description 6
- 231100000719 pollutant Toxicity 0.000 description 6
- LISFMEBWQUVKPJ-UHFFFAOYSA-N quinolin-2-ol Chemical compound C1=CC=C2NC(=O)C=CC2=C1 LISFMEBWQUVKPJ-UHFFFAOYSA-N 0.000 description 6
- 238000004064 recycling Methods 0.000 description 6
- 235000019364 tetracycline Nutrition 0.000 description 6
- 150000003522 tetracyclines Chemical class 0.000 description 6
- 150000003952 β-lactams Chemical class 0.000 description 6
- 238000003753 real-time PCR Methods 0.000 description 5
- 150000001412 amines Chemical class 0.000 description 4
- 238000005457 optimization Methods 0.000 description 4
- 244000052769 pathogen Species 0.000 description 4
- 229940056360 penicillin g Drugs 0.000 description 4
- 101150015970 tetM gene Proteins 0.000 description 4
- 229960002180 tetracycline Drugs 0.000 description 4
- 229930101283 tetracycline Natural products 0.000 description 4
- RXZBMPWDPOLZGW-XMRMVWPWSA-N (E)-roxithromycin Chemical compound O([C@@H]1[C@@H](C)C(=O)O[C@@H]([C@@]([C@H](O)[C@@H](C)C(=N/OCOCCOC)/[C@H](C)C[C@@](C)(O)[C@H](O[C@H]2[C@@H]([C@H](C[C@@H](C)O2)N(C)C)O)[C@H]1C)(C)O)CC)[C@H]1C[C@@](C)(OC)[C@@H](O)[C@H](C)O1 RXZBMPWDPOLZGW-XMRMVWPWSA-N 0.000 description 3
- PTNZGHXUZDHMIQ-UHFFFAOYSA-N 4-(dimethylamino)-1,5,10,11,12a-pentahydroxy-6-methyl-3,12-dioxo-4a,5,5a,6-tetrahydro-4h-tetracene-2-carboxamide;hydrochloride Chemical compound Cl.C1=CC=C2C(C)C(C(O)C3C(C(O)=C(C(N)=O)C(=O)C3N(C)C)(O)C3=O)C3=C(O)C2=C1O PTNZGHXUZDHMIQ-UHFFFAOYSA-N 0.000 description 3
- GSDSWSVVBLHKDQ-UHFFFAOYSA-N 9-fluoro-3-methyl-10-(4-methylpiperazin-1-yl)-7-oxo-2,3-dihydro-7H-[1,4]oxazino[2,3,4-ij]quinoline-6-carboxylic acid Chemical compound FC1=CC(C(C(C(O)=O)=C2)=O)=C3N2C(C)COC3=C1N1CCN(C)CC1 GSDSWSVVBLHKDQ-UHFFFAOYSA-N 0.000 description 3
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 3
- WMPXPUYPYQKQCX-UHFFFAOYSA-N Sulfamonomethoxine Chemical compound C1=NC(OC)=CC(NS(=O)(=O)C=2C=CC(N)=CC=2)=N1 WMPXPUYPYQKQCX-UHFFFAOYSA-N 0.000 description 3
- 239000002253 acid Substances 0.000 description 3
- 230000003115 biocidal effect Effects 0.000 description 3
- 229910052801 chlorine Inorganic materials 0.000 description 3
- 239000000460 chlorine Substances 0.000 description 3
- 229960003405 ciprofloxacin Drugs 0.000 description 3
- 229960002626 clarithromycin Drugs 0.000 description 3
- AGOYDEPGAOXOCK-KCBOHYOISA-N clarithromycin Chemical compound O([C@@H]1[C@@H](C)C(=O)O[C@@H]([C@@]([C@H](O)[C@@H](C)C(=O)[C@H](C)C[C@](C)([C@H](O[C@H]2[C@@H]([C@H](C[C@@H](C)O2)N(C)C)O)[C@H]1C)OC)(C)O)CC)[C@H]1C[C@@](C)(OC)[C@@H](O)[C@H](C)O1 AGOYDEPGAOXOCK-KCBOHYOISA-N 0.000 description 3
- 229960004082 doxycycline hydrochloride Drugs 0.000 description 3
- 229960003276 erythromycin Drugs 0.000 description 3
- 230000002779 inactivation Effects 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 229960001180 norfloxacin Drugs 0.000 description 3
- OGJPXUAPXNRGGI-UHFFFAOYSA-N norfloxacin Chemical compound C1=C2N(CC)C=C(C(O)=O)C(=O)C2=CC(F)=C1N1CCNCC1 OGJPXUAPXNRGGI-UHFFFAOYSA-N 0.000 description 3
- 229960001699 ofloxacin Drugs 0.000 description 3
- 229960005224 roxithromycin Drugs 0.000 description 3
- SEEPANYCNGTZFQ-UHFFFAOYSA-N sulfadiazine Chemical compound C1=CC(N)=CC=C1S(=O)(=O)NC1=NC=CC=N1 SEEPANYCNGTZFQ-UHFFFAOYSA-N 0.000 description 3
- 229960004306 sulfadiazine Drugs 0.000 description 3
- 229960005404 sulfamethoxazole Drugs 0.000 description 3
- 229950003874 sulfamonomethoxine Drugs 0.000 description 3
- 229940124530 sulfonamide Drugs 0.000 description 3
- 150000003456 sulfonamides Chemical class 0.000 description 3
- JLKIGFTWXXRPMT-UHFFFAOYSA-N sulphamethoxazole Chemical compound O1C(C)=CC(NS(=O)(=O)C=2C=CC(N)=CC=2)=N1 JLKIGFTWXXRPMT-UHFFFAOYSA-N 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- QYAPHLRPFNSDNH-MRFRVZCGSA-N (4s,4as,5as,6s,12ar)-7-chloro-4-(dimethylamino)-1,6,10,11,12a-pentahydroxy-6-methyl-3,12-dioxo-4,4a,5,5a-tetrahydrotetracene-2-carboxamide;hydrochloride Chemical compound Cl.C1=CC(Cl)=C2[C@](O)(C)[C@H]3C[C@H]4[C@H](N(C)C)C(=O)C(C(N)=O)=C(O)[C@@]4(O)C(=O)C3=C(O)C2=C1O QYAPHLRPFNSDNH-MRFRVZCGSA-N 0.000 description 2
- 150000007513 acids Chemical class 0.000 description 2
- LSQZJLSUYDQPKJ-NJBDSQKTSA-N amoxicillin Chemical compound C1([C@@H](N)C(=O)N[C@H]2[C@H]3SC([C@@H](N3C2=O)C(O)=O)(C)C)=CC=C(O)C=C1 LSQZJLSUYDQPKJ-NJBDSQKTSA-N 0.000 description 2
- 229960003022 amoxicillin Drugs 0.000 description 2
- 239000003782 beta lactam antibiotic agent Substances 0.000 description 2
- 230000000711 cancerogenic effect Effects 0.000 description 2
- 231100000315 carcinogenic Toxicity 0.000 description 2
- XMEVHPAGJVLHIG-FMZCEJRJSA-N chembl454950 Chemical compound [Cl-].C1=CC=C2[C@](O)(C)[C@H]3C[C@H]4[C@H]([NH+](C)C)C(O)=C(C(N)=O)C(=O)[C@@]4(O)C(O)=C3C(=O)C2=C1O XMEVHPAGJVLHIG-FMZCEJRJSA-N 0.000 description 2
- 239000000356 contaminant Substances 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 238000005286 illumination Methods 0.000 description 2
- 229940041033 macrolides Drugs 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- LSQZJLSUYDQPKJ-UHFFFAOYSA-N p-Hydroxyampicillin Natural products O=C1N2C(C(O)=O)C(C)(C)SC2C1NC(=O)C(N)C1=CC=C(O)C=C1 LSQZJLSUYDQPKJ-UHFFFAOYSA-N 0.000 description 2
- 150000007660 quinolones Chemical class 0.000 description 2
- 229940072172 tetracycline antibiotic Drugs 0.000 description 2
- 229960004989 tetracycline hydrochloride Drugs 0.000 description 2
- 229940040944 tetracyclines Drugs 0.000 description 2
- 239000002132 β-lactam antibiotic Substances 0.000 description 2
- 229940124586 β-lactam antibiotics Drugs 0.000 description 2
- OGQYJDHTHFAPRN-UHFFFAOYSA-N 2-fluoro-6-(trifluoromethyl)benzonitrile Chemical compound FC1=CC=CC(C(F)(F)F)=C1C#N OGQYJDHTHFAPRN-UHFFFAOYSA-N 0.000 description 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 1
- 241001465754 Metazoa Species 0.000 description 1
- 206010034133 Pathogen resistance Diseases 0.000 description 1
- 238000009825 accumulation Methods 0.000 description 1
- 230000004888 barrier function Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000006065 biodegradation reaction Methods 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 229960003185 chlortetracycline hydrochloride Drugs 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000010276 construction Methods 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 230000018109 developmental process Effects 0.000 description 1
- 239000003651 drinking water Substances 0.000 description 1
- 235000020188 drinking water Nutrition 0.000 description 1
- 229940079593 drug Drugs 0.000 description 1
- 239000003814 drug Substances 0.000 description 1
- 125000002485 formyl group Chemical class [H]C(*)=O 0.000 description 1
- 230000002068 genetic effect Effects 0.000 description 1
- 230000036541 health Effects 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 239000002207 metabolite Substances 0.000 description 1
- 230000002906 microbiologic effect Effects 0.000 description 1
- 231100000219 mutagenic Toxicity 0.000 description 1
- 230000003505 mutagenic effect Effects 0.000 description 1
- XKLJHFLUAHKGGU-UHFFFAOYSA-N nitrous amide Chemical compound ON=N XKLJHFLUAHKGGU-UHFFFAOYSA-N 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 235000019371 penicillin G benzathine Nutrition 0.000 description 1
- 230000005180 public health Effects 0.000 description 1
- 230000008929 regeneration Effects 0.000 description 1
- 238000011069 regeneration method Methods 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 231100000331 toxic Toxicity 0.000 description 1
- 230000002588 toxic effect Effects 0.000 description 1
- 210000002700 urine Anatomy 0.000 description 1
Images
Classifications
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
- C02F1/32—Treatment of water, waste water, or sewage by irradiation with ultraviolet light
-
- 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
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
- C02F1/722—Oxidation by peroxides
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/34—Organic compounds containing oxygen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/38—Organic compounds containing nitrogen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/40—Organic compounds containing sulfur
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2303/00—Specific treatment goals
- C02F2303/04—Disinfection
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/02—Specific form of oxidant
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/02—Specific form of oxidant
- C02F2305/023—Reactive oxygen species, singlet oxygen, OH radical
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W10/00—Technologies for wastewater treatment
- Y02W10/30—Wastewater or sewage treatment systems using renewable energies
- Y02W10/37—Wastewater or sewage treatment systems using renewable energies using solar energy
Landscapes
- 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)
- Health & Medical Sciences (AREA)
- Toxicology (AREA)
- Treatment Of Water By Oxidation Or Reduction (AREA)
- Physical Water Treatments (AREA)
Abstract
The invention belongs to the technical field of sewage treatment, and particularly discloses a method for removing antibiotics and resistance genes in sewage by using ultraviolet/peroxyacetic acid, wherein the peroxyacetic acid is added into the sewage, the mixture is uniformly stirred, and then the ultraviolet irradiation is carried out, so that the antibiotics and the resistance genes in the sewage can be simultaneously removed: the reaction temperature is not limited, the dosage of the peroxyacetic acid is 3-8 mg/L, and the radiation wavelength of an ultraviolet lamp is 300 mu W/cm2The dose of ultraviolet is 36-180 mJ/cm2And the reaction time is 1-10 min. The method can remove broad-spectrum antibiotics and resistance genes in sewage simultaneously, does not produce secondary pollution, has mild reaction conditions, short treatment process time, is simple and easy to implement, and is suitable for antibiotics and resistance genesThe removal efficiency is high. The method is suitable for efficiently removing antibiotics and resistance genes in the sewage, can be used as a novel disinfection process to be applied to a sewage treatment plant, and has a wide application prospect.
Description
Technical Field
The invention relates to the technical field of sewage treatment, in particular to a method for removing antibiotics and resistance genes in sewage by using ultraviolet/peroxyacetic acid.
Background
With the increasing global water resource situation, sewage recycling has become an important strategy for solving water resource shortage in countries of the world. In some developed countries, the recycling of sewage starts earlier, and the sewage is well popularized and applied at present; and the development space of China is still quite large after the start of China. In the process of recycling sewage, public health and safety of recycled water are always concerned, and disinfection as a final barrier plays a crucial role in guaranteeing the recycling safety of sewage. Among them, effective inactivation of pathogens is a microbiological indicator that needs to be guaranteed during disinfection. However, with the increasing awareness of pollutants in sewage and the continuous progress of analytical detection means, it is found that more and more new pollutants are frequently detected in sewage in addition to traditional pollutants including pathogens, which also brings great challenges to the safe recycling of sewage.
The variety of emerging contaminants in sewage is diverse, with antibiotics being identified as emerging contaminants that require significant attention due to their widespread use and possible significant impact on human health and the environment. After being ingested by people and animals, most of antibiotics still can be discharged out of the body along with urine and excrement in the form of parent bodies or metabolites, and many of the antibiotics are poor in biodegradation and still exist in effluent after sewage treatment, so that great safety risk is brought to the recycling of the sewage. Antibiotics which are widely used at present are classified into β -lactams, sulfonamides, macrolides, quinolones, tetracyclines and the like according to chemical structures. In addition, the constant accumulation of Antibiotic drugs remaining in the environment increases bacterial resistance to induce Antibiotic resistance genetic factors, i.e., Antibiotic Resistance Genes (ARGs), that produce antibiotics. Recent studies have shown that ARGs are also an important class of emerging pollutants. Therefore, on the basis of ensuring the effective inactivation of pathogens in sewage, emerging pollutants are enhanced, and the removal of antibiotics and the ARGs thereof is very important in the field of sewage disinfection.
Among the conventional disinfection processes, chlorine disinfection is widely used in the disinfection treatment of sewage and drinking water. However, chlorine disinfection produces significant amounts of halogenated disinfection by-products such as trihalomethanes, haloacetic acids, haloacetonitrile, and haloaldehydes, among others. Nitrosamine disinfection byproducts are considered suspect carcinogenic compounds by the U.S. environmental protection agency because they are more carcinogenic and mutagenic than traditional halogenated disinfection byproducts such as trihalomethanes and haloacetic acids. The UV disinfection generates few disinfection byproducts and has good inactivation effect on pathogens, so the UV disinfection is considered to be a relatively effective disinfection process. However, UV disinfection is selective for removing refractory organics in wastewater, and the removal effect of ARGs is not ideal, which can cause the ARGs to generate a photo-revivification phenomenon. Therefore, the combination of UV and other disinfection processes which also produce few disinfection byproducts is an effective way for removing new pollutants such as antibiotics, resistance genes and the like in sewage. At present, no method for simultaneously removing a plurality of antibiotics and resistance genes in sewage economically and effectively exists.
Disclosure of Invention
The invention aims to provide a method for removing antibiotics and resistance genes in sewage by using ultraviolet/peroxyacetic acid, which solves the problems in the prior art, ensures that the reaction conditions for removing the sewage are simple and easy, the treatment effect is good, the reaction is mild, no secondary pollution is caused, the treatment cost is low, the industrial application prospect is wide, and various antibiotics and resistance genes in the sewage can be removed simultaneously.
In order to achieve the purpose, the invention provides the following scheme: the invention provides a method for synchronously removing antibiotics and resistance genes in sewage, which comprises the following steps:
(1) adding peracetic acid (PAA) into sewage, and then uniformly stirring to obtain a first mixed liquid;
(2) and (2) carrying out Ultraviolet (UV) irradiation on the first mixed liquid obtained in the step (1), so that antibiotics and resistance genes in the sewage can be removed simultaneously.
As a further optimization of the invention, the concentration of the peroxyacetic acid in the first mixed liquid in the step (1) is 3-8 mg/L.
As a further optimization of the present invention, the optimum concentration of peroxyacetic acid in the first mixed liquid in step (1) is 5 mg/L.
As a further optimization of the invention, in the step (2), the ultraviolet irradiation is carried out at the ultraviolet lamp radiation wavelength of 300 mu W/cm2The dose of ultraviolet is 36-180 mJ/cm2Irradiating for 1-10 min under the condition.
As a further optimization of the invention, in the step (2), the ultraviolet irradiation is carried out at the ultraviolet lamp radiation wavelength of 300 mu W/cm2The ultraviolet dose is 108mJ/cm2Irradiating for 6min under the condition.
The invention also provides application of the method for synchronously removing the antibiotics and the resistance genes in the sewage in sewage treatment.
The invention is suitable for treating sewage containing various antibiotics and resistance genes, including tetracyclines, sulfonamides, quinolones, macrolides, beta-lactams and the like. The invention is different from chlorine disinfection to generate a large amount of halogenated disinfection byproducts (trihalomethane, haloacetic acid, haloacetonitrile, halogenated aldehyde and the like), can effectively avoid the generation of toxic byproducts by adopting ultraviolet and peroxyacetic acid disinfection, is a novel environment-friendly sewage disinfection mode, and is beneficial to the regeneration and reuse of sewage.
In the prior art, only a small amount of active free radicals can be generated by single ultraviolet irradiation or only adding peroxyacetic acid. The method combines the two, the peracetic acid is added into the sewage, the ultraviolet irradiation is assisted, the reaction temperature is not limited, an additional heating device is not needed, the reaction time is only 1-10 min, the peracetic acid can be quickly activated by the ultraviolet irradiation in the reaction process, so that more hydroxyl radicals are generated, carbon-containing radicals are generated, the oxidation effect is effectively improved, and the highest removal rate of antibiotics and resistance genes can reach 100%. And the peroxyacetic acid is cheap and easy to obtain, the dosage of the used ultraviolet is low, and the construction cost and the operation cost of the invention are low.
The invention discloses the following technical effects:
(1) the invention provides a method for removing antibiotics and resistance genes in sewage by using ultraviolet/peroxyacetic acid, which has a wide target object application range and can simultaneously remove various antibiotics and resistance genes.
(2) The method has the advantages of mild reaction conditions, high removal rate, simple and easy reaction conditions, short treatment time, no generation of disinfection byproducts, environmental friendliness, low treatment cost and good application prospect.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings needed to be used in the embodiments will be briefly described below, and it is obvious that the drawings in the following description are only some embodiments of the present invention, and it is obvious for those skilled in the art to obtain other drawings without inventive exercise.
FIG. 1 is a graph showing the calculation results of the removal rates of tetracycline hydrochloride, chlortetracycline hydrochloride and doxycycline hydrochloride in sewage in examples 1-2 and comparative examples 1-3 of Experimental example 1;
FIG. 2 is the calculation results of the removal rates of sulfadiazine, sulfamethoxazole and sulfamonomethoxine in sewage in examples 1-2 and comparative examples 1-3 of Experimental example 2;
FIG. 3 is a graph showing the calculation results of the removal rates of ciprofloxacin, ofloxacin and norfloxacin from wastewater in examples 1 to 2 and comparative examples 1 to 3 of Experimental example 3;
FIG. 4 is a graph showing the results of calculation of the removal rates of roxithromycin, erythromycin and clarithromycin from sewage in examples 1-2 and comparative examples 1-3 of Experimental example 4;
FIG. 5 shows the calculation results of the salt removal rates of benzylpenicillin and penicillin G in the wastewater of examples 1-2 and comparative examples 1-3 in Experimental example 5;
FIG. 6 is a calculation result of the removal rate of the tetracycline resistance gene tetM in the sewage in examples 1 to 2 and comparative examples 1 to 3 in Experimental example 6;
FIG. 7 is a calculation result of the removal rate of amine resistance gene sul3 in sewage in examples 1-2 and comparative examples 1-3 of Experimental example 7;
FIG. 8 is a calculation result of the removal rate of the quinolone resistance gene qnrD from the sewage in examples 1 to 2 and comparative examples 1 to 3 in Experimental example 8;
FIG. 9 is a calculation result of the removal rate of the macrolide resistance gene ermA in sewage in examples 1 to 2 and comparative examples 1 to 3 in experimental example 9;
FIG. 10 shows examples 1 to 2 and comparative examples 1 to 3 in Experimental example 10 for the beta-lactam resistance gene bla in wastewaterOXA1And calculating the removal rate.
Detailed Description
Reference will now be made in detail to various exemplary embodiments of the invention, the detailed description should not be construed as limiting the invention but as a more detailed description of certain aspects, features and embodiments of the invention.
It is to be understood that the terminology used herein is for the purpose of describing particular embodiments only and is not intended to be limiting of the invention. Further, for numerical ranges in this disclosure, it is understood that each intervening value, between the upper and lower limit of that range, is also specifically disclosed. Every smaller range between any stated value or intervening value in a stated range and any other stated or intervening value in a stated range is encompassed within the invention. The upper and lower limits of these smaller ranges may independently be included or excluded in the range.
Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. Although only preferred methods and materials are described herein, any methods and materials similar or equivalent to those described herein can be used in the practice or testing of the present invention. All documents mentioned in this specification are incorporated by reference herein for the purpose of disclosing and describing the methods and/or materials associated with the documents. In case of conflict with any incorporated document, the present specification will control.
It will be apparent to those skilled in the art that various modifications and variations can be made in the specific embodiments of the present disclosure without departing from the scope or spirit of the disclosure. Other embodiments will be apparent to those skilled in the art from consideration of the specification. The description and examples are intended to be illustrative only.
As used herein, the terms "comprising," "including," "having," "containing," and the like are open-ended terms that mean including, but not limited to.
Example 1
Taking actual secondary effluent sewage of a sewage treatment plant, adding a peroxyacetic acid solution into the sewage, uniformly mixing to obtain a first mixed liquid, wherein the peroxyacetic acid concentration in the first mixed liquid is 3mg/L, and the radiation wavelength of the first mixed liquid under an ultraviolet lamp is 300 mu W/cm2The ultraviolet dose is 36mJ/cm2Irradiating for 2min under the condition, wherein the mark group is a UV/PAA-L group.
Example 2
Taking actual secondary effluent of a sewage treatment plant as sewage, adding a peroxyacetic acid solution into the sewage, uniformly mixing to obtain a first mixed liquid, wherein the peroxyacetic acid concentration in the first mixed liquid is 5mg/L, and radiating the first mixed liquid by an ultraviolet lamp at a wavelength of 300 mu W/cm2The ultraviolet dose is 108mJ/cm2Irradiating for 6min under the condition, wherein the mark group is a UV/PAA-H group.
Comparative example 1
Taking actual secondary effluent of a sewage treatment plant as sewage, treating the sewage only by using an ultraviolet disinfection mode alone, and treating the sewage under the condition that the ultraviolet light intensity is 300 mu W/cm2The ultraviolet dose is 36mJ/cm2The illumination time is 2min under the condition, and the mark group is UV-L group.
Comparative example 2
Taking actual secondary effluent sewage of a sewage treatment plant, treating the sewage only by using an ultraviolet disinfection mode alone, and treating the sewage at the ultraviolet light intensity of 300 mu W/cm2The ultraviolet dose is 180mJ/cm2The illumination time under the condition is 10min, and the mark group is UV-H group.
Comparative example 3
Taking actual secondary effluent sewage of a sewage treatment plant, treating the sewage only by using a peroxyacetic acid disinfection mode alone, adding a diluted peroxyacetic acid solution into the sewage to enable the concentration of the peroxyacetic acid in the sewage to be 8mg/L, reacting for 30min, and marking the group as a PAA group.
Experimental example 1
By measuring the concentrations of tetracycline antibiotics tetracycline hydrochloride, aureomycin hydrochloride and doxycycline hydrochloride in the actual secondary effluent of the sewage treatment plants in the examples 1-2 and the comparative examples 1-3 before and after sewage treatment, the removal rates of the hydrochloride, aureomycin hydrochloride and doxycycline hydrochloride in different sewage treatment modes are calculated, and the graph 1 is obtained.
By the aid of the graph 1, the ultraviolet/peracetic acid combined sewage treatment method can be used, and the removal efficiency of the three tetracycline antibiotics can reach 100%.
Experimental example 2
By measuring the concentrations of sulfa antibiotics sulfadiazine, sulfamethoxazole and sulfamonomethoxine in the actual secondary effluent of the sewage treatment plants in the examples 1-2 and the comparative examples 1-3 before and after sewage treatment, the removal rates of sulfadiazine, sulfamethoxazole and sulfamonomethoxine under different sewage treatment modes are calculated, and the graph 2 is obtained.
By using the ultraviolet/peracetic acid combination for sewage treatment, the best removal effect on the three sulfonamides antibiotics can be obtained by using the figure 2, and the average removal rate is 35% and can reach 52% at most.
Experimental example 3
By measuring the concentrations of the quinolone antibiotics ciprofloxacin, ofloxacin and norfloxacin before and after sewage treatment in the actual secondary effluent of the sewage treatment plants in examples 1-2 and comparative examples 1-3, the removal rates of ciprofloxacin, ofloxacin and norfloxacin in different sewage treatment modes are calculated, and a graph 3 is obtained.
By the aid of the graph 3, the ultraviolet/peracetic acid combined sewage treatment method has the best effect of removing the three quinolone antibiotics, and the average removal rate is 93.9% and is 100% at most.
Experimental example 4
By measuring the concentrations of the macrolide antibiotics roxithromycin, erythromycin and clarithromycin in the actual secondary effluent of the sewage treatment plants in examples 1-2 and comparative examples 1-3 before and after sewage treatment, the removal rates of roxithromycin, erythromycin and clarithromycin in different sewage treatment modes are calculated, and a graph 4 is obtained.
By using the graph of FIG. 4, it can be shown that the ultraviolet/peracetic acid combined sewage treatment method has the best effect of removing three macrolide antibiotics, and the average removal rate is 25.7% and the maximum removal rate is 29.3%.
Experimental example 5
By measuring the concentrations of the beta-lactam antibiotics amoxicillin and penicillin G methyl salt in the actual secondary effluent of the sewage treatment plants in the examples 1-2 and the comparative examples 1-3 before and after sewage treatment, the removal rates of the amoxicillin and penicillin G methyl salt in different sewage treatment modes are calculated, and the graph 5 is obtained.
By using the ultraviolet/peracetic acid combined sewage treatment process shown in fig. 5, the best removal effect of the two beta-lactam antibiotics can be achieved, and the average removal rate is 95.6% and is 100% at most.
Experimental example 6
The abundance of the tetracycline resistance gene tetM in the actual secondary effluent of the sewage treatment plants in examples 1-2 and comparative examples 1-3 before and after sewage treatment was measured by real-time fluorescent quantitative PCR, and the removal rate of the tetracycline resistance gene tetM in the sewage in different sewage treatment modes was calculated, to obtain fig. 6.
The figure 6 shows that the ultraviolet/peracetic acid combined sewage treatment has the best effect of removing the tetracycline resistance gene tetM, and the highest effect is 37.1%.
Experimental example 7
The abundance of the amine resistance gene sul3 in the actual secondary effluent of the sewage treatment plants in examples 1-2 and comparative examples 1-3 before and after sewage treatment is measured by real-time fluorescent quantitative PCR, and the removal rate of the amine resistance gene sul3 in sewage in different sewage treatment modes is calculated, so that the graph of fig. 7 is obtained.
The figure 7 shows that the ultraviolet/peracetic acid combined sewage treatment has the best effect of removing the amine resistance gene sul3, and the maximum effect is 64.3%.
Experimental example 8
The abundance of the quinolone resistance gene qnrD in the actual secondary effluent of the sewage treatment plants in examples 1-2 and comparative examples 1-3 before and after sewage treatment was measured by real-time fluorescent quantitative PCR, and the removal rate of the quinolone resistance gene qnrD in the sewage in different sewage treatment modes was calculated, so that fig. 8 was obtained.
The figure 8 shows that the ultraviolet/peroxyacetic acid combined sewage treatment has the best effect of removing the quinolone resistant gene qnrD, and the maximum effect is 52.5%.
Experimental example 9
The abundance of the macrolide resistance gene ermA in the actual secondary effluent of the sewage treatment plants in examples 1-2 and comparative examples 1-3 before and after sewage treatment was measured by real-time fluorescent quantitative PCR, and the removal rate of the macrolide resistance gene ermA in the sewage in different sewage treatment modes was calculated, thus obtaining FIG. 9.
FIG. 9 shows that the ultraviolet/peracetic acid combined sewage treatment has the best effect of removing the macrolide resistance gene ermA, and the maximum effect is 100%.
Experimental example 10
Determination of the beta-lactam resistance Gene bla in actual Secondary effluent from Sewage treatment plants in examples 1-2 and comparative examples 1-3 by real-time fluorescent quantitative PCROXA1The abundance before and after the sewage treatment is carried out, and the beta-lactam resistance gene bla in the sewage in different sewage treatment modes is calculatedOXA1The removal rate was found to be FIG. 10.
FIG. 10 shows that the beta-lactam resistance gene bla is treated by the UV/peracetic acid combination for wastewater treatmentOXA1The removal effect of (a) is the best, and the maximum is 30.2%.
The above-described embodiments are merely illustrative of the preferred embodiments of the present invention, and do not limit the scope of the present invention, and various modifications and improvements of the technical solutions of the present invention can be made by those skilled in the art without departing from the spirit of the present invention, and the technical solutions of the present invention are within the scope of the present invention defined by the claims.
Claims (6)
1. The method for removing antibiotics and resistance genes in sewage by using ultraviolet/peroxyacetic acid is characterized by comprising the following steps of:
(1) adding peroxyacetic acid into sewage, and then uniformly stirring to obtain a first mixed liquid;
(2) and (2) carrying out ultraviolet irradiation on the first mixed liquid obtained in the step (1), so that antibiotics and resistance genes in the sewage can be removed simultaneously.
2. The method for removing antibiotics and resistance genes in sewage by using ultraviolet/peroxyacetic acid as claimed in claim 1, wherein the concentration of the peroxyacetic acid in the first mixed liquid in the step (1) is 3-8 mg/L.
3. The method for removing antibiotics and resistance genes in sewage by using ultraviolet/peroxyacetic acid as claimed in claim 2, wherein the concentration of peroxyacetic acid in the first mixed liquid in the step (1) is 5 mg/L.
4. The method for removing antibiotics and resistance genes in sewage by using ultraviolet/peroxyacetic acid as claimed in claim 1, wherein the ultraviolet irradiation in step (2) is at ultraviolet lamp irradiation wavelength of 300 μ W/cm2The dose of ultraviolet is 36-180 mJ/cm2Irradiating for 1-10 min under the condition.
5. The method for removing antibiotics and resistance genes in sewage by using ultraviolet/peroxyacetic acid as claimed in claim 4, wherein the ultraviolet irradiation in step (2) is at ultraviolet lamp irradiation wavelength of 300 μ W/cm2The ultraviolet dose is 108mJ/cm2Irradiating for 6min under the condition.
6. Use of the method for simultaneous removal of antibiotics and resistance genes from wastewater according to claim 1 in wastewater treatment.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202111152435.4A CN113896276B (en) | 2021-09-29 | 2021-09-29 | Method for removing antibiotics and resistance genes in sewage by using ultraviolet/peroxyacetic acid |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202111152435.4A CN113896276B (en) | 2021-09-29 | 2021-09-29 | Method for removing antibiotics and resistance genes in sewage by using ultraviolet/peroxyacetic acid |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN113896276A true CN113896276A (en) | 2022-01-07 |
| CN113896276B CN113896276B (en) | 2023-02-07 |
Family
ID=79189213
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN202111152435.4A Active CN113896276B (en) | 2021-09-29 | 2021-09-29 | Method for removing antibiotics and resistance genes in sewage by using ultraviolet/peroxyacetic acid |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN113896276B (en) |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115321637A (en) * | 2022-08-24 | 2022-11-11 | 北京工业大学 | Method for removing antibiotic resistance genes by vacuum ultraviolet/potassium hydrogen persulfate coupled advanced oxidation and regulation and control system |
| CN117069199A (en) * | 2023-08-22 | 2023-11-17 | 同济大学 | Application of riboflavin-mediated ultraviolet/peracetic acid-enhanced H2 receptor antagonist in water |
Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US20140124440A1 (en) * | 2012-03-29 | 2014-05-08 | Nanjing University | Method for removing genes encoding antibiotic resistance |
| CN111620493A (en) * | 2020-07-03 | 2020-09-04 | 中国农业科学院农业环境与可持续发展研究所 | Method and special equipment for removing antibiotic resistant bacteria and resistant genes in sewage |
| CN111792719A (en) * | 2019-07-30 | 2020-10-20 | 哈尔滨工业大学 | Oxidation method for removing antibiotic resistance genes and resistant bacteria in sewage |
| CN112142182A (en) * | 2020-08-24 | 2020-12-29 | 同济大学 | Removal and application of ultraviolet/peroxyacetic acid to refractory antibiotics in town sewage |
| CN113415869A (en) * | 2021-05-27 | 2021-09-21 | 同济大学 | Method for synergistically degrading refractory organic matters in town sewage by using hydrogen peroxide component in low-concentration peroxyacetic acid |
-
2021
- 2021-09-29 CN CN202111152435.4A patent/CN113896276B/en active Active
Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US20140124440A1 (en) * | 2012-03-29 | 2014-05-08 | Nanjing University | Method for removing genes encoding antibiotic resistance |
| CN111792719A (en) * | 2019-07-30 | 2020-10-20 | 哈尔滨工业大学 | Oxidation method for removing antibiotic resistance genes and resistant bacteria in sewage |
| CN111620493A (en) * | 2020-07-03 | 2020-09-04 | 中国农业科学院农业环境与可持续发展研究所 | Method and special equipment for removing antibiotic resistant bacteria and resistant genes in sewage |
| CN112142182A (en) * | 2020-08-24 | 2020-12-29 | 同济大学 | Removal and application of ultraviolet/peroxyacetic acid to refractory antibiotics in town sewage |
| CN113415869A (en) * | 2021-05-27 | 2021-09-21 | 同济大学 | Method for synergistically degrading refractory organic matters in town sewage by using hydrogen peroxide component in low-concentration peroxyacetic acid |
Non-Patent Citations (1)
| Title |
|---|
| 韩中兴: "《现代医用消毒与医院感染控制技术 上》", 31 August 2019, 吉林科学技术出版社 * |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115321637A (en) * | 2022-08-24 | 2022-11-11 | 北京工业大学 | Method for removing antibiotic resistance genes by vacuum ultraviolet/potassium hydrogen persulfate coupled advanced oxidation and regulation and control system |
| CN115321637B (en) * | 2022-08-24 | 2023-09-22 | 北京工业大学 | Method and regulation and control system for removing antibiotic resistance gene by coupling vacuum ultraviolet/potassium hydrogen persulfate with advanced oxidation |
| CN117069199A (en) * | 2023-08-22 | 2023-11-17 | 同济大学 | Application of riboflavin-mediated ultraviolet/peracetic acid-enhanced H2 receptor antagonist in water |
| CN117069199B (en) * | 2023-08-22 | 2024-03-22 | 同济大学 | Application of riboflavin-mediated ultraviolet/peracetic acid-enhanced H2 receptor antagonist in water |
Also Published As
| Publication number | Publication date |
|---|---|
| CN113896276B (en) | 2023-02-07 |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| Ding et al. | UV photolysis as an efficient pretreatment method for antibiotics decomposition and their antibacterial activity elimination | |
| CN113896276B (en) | Method for removing antibiotics and resistance genes in sewage by using ultraviolet/peroxyacetic acid | |
| Wang et al. | The occurrence, distribution and degradation of antibiotics by ionizing radiation: an overview | |
| Carbajo et al. | Continuous ozonation treatment of ofloxacin: transformation products, water matrix effect and aquatic toxicity | |
| Michael et al. | Investigating the impact of UV-C/H2O2 and sunlight/H2O2 on the removal of antibiotics, antibiotic resistance determinants and toxicity present in urban wastewater | |
| Lofrano et al. | Advanced oxidation processes for antibiotics removal: a review | |
| Kurt et al. | Treatment of antibiotics in wastewater using advanced oxidation processes (AOPs) | |
| Rozas et al. | Experimental design of Fenton and photo-Fenton reactions for the treatment of ampicillin solutions | |
| Malvestiti et al. | Disinfection of secondary effluents by O3, O3/H2O2 and UV/H2O2: Influence of carbonate, nitrate, industrial contaminants and regrowth | |
| García-Muñoz et al. | Treatment of hospital wastewater through the CWPO-Photoassisted process catalyzed by ilmenite | |
| Norabadi et al. | Optimizing the parameters of amoxicillin removal in a photocatalysis/ozonation process using Box-Behnken response surface methodology | |
| Akpotu et al. | Photocatalysis and biodegradation of pharmaceuticals in wastewater: effect of abiotic and biotic factors | |
| Bobu et al. | Comparison of different advanced oxidation processes for the degradation of two fluoroquinolone antibiotics in aqueous solutions | |
| Beretsou et al. | A chemical, microbiological and (eco) toxicological scheme to understand the efficiency of UV-C/H2O2 oxidation on antibiotic-related microcontaminants in treated urban wastewater | |
| Zouanti et al. | Experimental study of degradation and biodegradability of oxytetracycline antibiotic in aqueous solution using Fenton process | |
| Rizzo | Addressing main challenges in the tertiary treatment of urban wastewater: are homogeneous photodriven AOPs the answer? | |
| Serrano et al. | Efficient removal of the pharmaceutical pollutants included in the EU Watch List (Decision 2015/495) by modified magnetite/H2O2 | |
| CN103212410A (en) | Catalyst, preparation method of catalyst and water treatment device containing catalyst | |
| Rasoulifard et al. | Photocatalytic degradation of tylosin via ultraviolet-activated persulfate in aqueous solution | |
| Huang et al. | Radiation-induced degradation of sulfonamide and quinolone antibiotics: A brief review | |
| Boudriche et al. | UV‐C‐driven oxidation of ciprofloxacin in conventionally treated urban wastewater: degradation kinetics, ecotoxicity and phytotoxicity assessment and inactivation of ciprofloxacin‐resistant Escherichia coli | |
| Terefinko et al. | Removal of clinically significant antibiotics from aqueous solutions by applying unique high-throughput continuous-flow plasma pencil and plasma brush systems | |
| CN112777820A (en) | Method for cooperatively controlling microorganisms and disinfection byproducts in effluent of sewage treatment plant | |
| Azuma et al. | Inactivation of antibiotic-resistant bacteria in hospital wastewater by ozone-based advanced water treatment processes | |
| Fanourgiakis et al. | Simultaneous removal of estrogens and pathogens from secondary treated wastewater by solar photocatalytic treatment |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| PB01 | Publication | ||
| PB01 | Publication | ||
| SE01 | Entry into force of request for substantive examination | ||
| SE01 | Entry into force of request for substantive examination | ||
| GR01 | Patent grant | ||
| GR01 | Patent grant |