發(fā)布時間：2018-04-12 17:25

  本文選題：氟喹諾酮 + 吸附　； 參考：《東華大學》2017年碩士論文

【摘要】：氟喹諾酮類抗生素是畜牧養(yǎng)殖業(yè)中廣泛使用的廣譜性抗菌劑�？股厥┯糜趧游锖�,60-90%以抗生素原藥或代謝物的形式經動物排泄物排出,對地表水、土壤、沉積物、地下水等造成污染,影響動物、植物和微生物的正常生命活動,并通過食物鏈最終影響人類的健康�？股氐目剐曰驅儆谛滦铜h(huán)境污染物,其危害風險較抗生素本身更嚴重更復雜。本文通過對集約化養(yǎng)殖場污染場地中氟喹諾酮類抗生素的調查、污染途徑分析與控制實驗,進行了抗生素及其抗性基因的風險評價,為控制抗生素及抗性基因的污染提供科學依據。開展環(huán)境中氟喹諾酮類抗生素的生態(tài)風險、污染行為及控制技術的研究具有重要的意義。本文研究結論如下:(1)利用物種敏感性評價方法得到的諾氟沙星、環(huán)丙沙星、恩諾沙星的在地表水中的預計無影響濃度(PNEC)分別為ρ(諾氟沙星)2.66μg/L、ρ(環(huán)丙沙星)9.92μg/L、ρ(恩諾沙星)5.11μg/L;根據物種敏感性分布評價結果利用風險熵值法RQ=PEC/PNEC評價中國地表水體的氟喹諾酮類抗生素污染風險。結果表明:除黃河、渤海灣、大遼河地表水中諾氟沙星的風險為低風險以外,地表水中氟喹諾酮的污染分布無風險。地表水急性水質基準CMC分別為:ρ(諾氟沙星)5.39μg/L、ρ(環(huán)丙沙星)20.10μg/L,ρ(恩諾沙星)11.16μg/L,慢性水質標準ccc分別為ρ(諾氟沙星)2.66μg/l、ρ(環(huán)丙沙星)9.92μg/l,ρ(恩諾沙星)5.51μg/l,以期為建立抗生素地表水環(huán)境質量標準提供參考。(2)利用評價因子法得到的諾氟沙星、環(huán)丙沙星、恩諾沙星在土壤環(huán)境中的pnec分別為11.30μg/kg、1.13μg/kg、45.00μg/kg。根據評價因子法結果利用風險熵值rq=pec/pnec評價了山東菜地、東莞菜地、福建養(yǎng)殖場周邊土壤環(huán)丙沙星均表現(xiàn)為高風險,應該重點監(jiān)控。山東菜地、東莞菜地諾氟沙星為中等風險,恩諾沙星為低風險。(3)在綜合分析抗性基因的產生過程、傳播途徑、基因降解及抗性細菌的耐藥程度等基礎上,提出“漸變-累積-突變”理論,建立了抗性基因的風險評價體系。通過危害識別、暴露評估、風險表征3個步驟,其中暴露評估將綜合風險分為4個指數(shù)來分別評價:抗性指數(shù)、傳播指數(shù)、污染指數(shù)、降解指數(shù)。通過分別對每個指數(shù)進行評分計算,將分值乘以權重后相加得到綜合風險,對風險進行分級,得到相對風險等級1-5級。(4)諾氟沙星、環(huán)丙沙星、恩諾沙星在三種不同場地介質中的吸附動力學均符合準二級動力學方程,其中在有機肥的影響下,三種氟喹諾酮類抗生素的吸附速率加快。其中環(huán)丙沙星更容易被吸附,三種氟喹諾酮類抗生素的遷移能力cipnorenr。在三種場地介質中諾氟沙星、環(huán)丙沙星、恩諾沙星的吸附熱力學符合freundlich模型,屬于物理吸附。三種介質中的吸附行為差異明顯。其土壤kf值分別為:47.4679、47.2607、33.9860;土壤+糞便kf值分別為:81.4329、90.1779、46.2594;土壤+有機肥kf值分別為:128.0855、133.5365、64.0914。(5)通過土柱淋溶實驗,在40天試驗時間中,土柱內抗生素未見明顯淋出,且三種初始濃度不同污染溶液對土柱中抗生素淋出情況并無影響,三種不同氟喹諾酮類抗生素的淋出行為相似。原因在于諾氟沙星、環(huán)丙沙星、恩諾沙星的吸附系數(shù)大,土壤黏度較大,一部分的抗生素被土壤吸附,三種抗生素的半衰期較短,一部分自身降解,由于土壤環(huán)境中存在微生物,不排除被微生物降解的可能性。土柱實驗結果表明:當抗生素未經處理直接排放到土壤中時,在短時間內會在土壤中積累,由于抗生素自身的水解等作用且與土壤結合,不會導致地下水的污染,但是長時間低劑量的暴露會誘導土壤中抗性基因的產生,從而形成抗性細菌,當抗性基因通過水平擴散等作用實現(xiàn)在不同種微生物之間的傳播,誘導超級細菌的產生。因此需要預防抗生素進入土壤環(huán)境。(6)通過木屑、稻谷殼、稻谷炭、顆粒活性炭等吸附實驗,表明活性炭對諾氟沙星、環(huán)丙沙星、恩諾沙星吸附效果最好,去除率均達到90%以上�；钚蕴繉θN氟喹諾酮類抗生素的吸附符合準二級吸附動力學,反應時間60min左右,三種氟喹諾酮類抗生素基本達到吸附平衡,其中活性炭對恩諾沙星的單位吸附平衡量最大,可達到2000mg/kg;活性炭對三種氟喹諾酮類抗生素的吸附符合freundlich吸附模型,屬于物理吸附過程,kf值分別為諾氟沙星1148.9735、環(huán)丙沙星1115.8351、恩諾沙星1200.3835。通過超聲再生活性炭實驗表明,在超聲進行到25 min時超聲再生效率達到最大,諾氟沙星、環(huán)丙沙星、恩諾沙星分別為68.5%、68.0%、69.9%;當溫度為35℃時超聲再生活性炭的再生效率最高,諾氟沙星、環(huán)丙沙星、恩諾沙星分別為73.1%、72.7%、73.6%;當超聲的頻率為40 KHz時,超聲對活性炭的再生效率最高,諾氟沙星、環(huán)丙沙星、恩諾沙星分別為76.5%、75.4%、79.0%。
[Abstract]:Fluoroquinolones are broad-spectrum antibiotics widely used in animal husbandry. Antibiotics antibacterial agent applied to animal, 60-90% to antibiotics or metabolites in the form of the original animal excrement discharged to surface water, soil, sediment, groundwater pollution, affect the normal life activities of animals, plants and microorganisms, and through the food chain the final impact on human health. The antibiotic resistance gene is a new type of environmental pollutants, the risk is more serious and more complex. The antibiotic itself through investigation of intensive farms contaminated sites of fluorine in quinolone antibiotics, pollution analysis and control experiment for the risk assessment and its antibiotic resistance genes, to provide scientific basis for for the control of antibiotic resistance genes and pollution. To carry out the ecological risk of fluoroquinolone antibiotics in the environment, pollution behavior and control technology It has important meaning to research. The conclusions of this study are as follows: (1) ciprofloxacin using species sensitivity evaluation method of norfloxacin, enrofloxacin, is expected in the surface water had no effect concentration (PNEC) respectively, P (norfloxacin) 2.66 g/L, P (Huan Bingsha) 9.92 g/L, P (enrofloxacin) 5.11 g/L; evaluation of fluoroquinolone antibiotics pollution risk Chinese surface water according to the evaluation results using species sensitivity distribution risk entropy method RQ=PEC/PNEC. The results showed that: in addition to the Yellow River, the Gulf of Bohai, the risk in surface water norfloxacin as low risk, fluoroquinolones in surface water pollution distribution without the risk of surface water quality criteria for acute CMC. Respectively: P (norfloxacin) 5.39 g/L, P (ciprofloxacin) 20.10 g/L, P (enrofloxacin) 11.16 g/L, chronic water quality standard CCC were p (norfloxacin) 2.66 g/l, P (ciprofloxacin) 9.92 g/ L, P (enrofloxacin) 5.51 g/l, in order to provide reference for the establishment of environmental quality standards for surface water antibiotics. (2) obtained by factor analysis of ciprofloxacin, norfloxacin, enrofloxacin PNEC in soil were 11.30 g/kg, 1.13 g/kg, 45 g/kg. according to the factor analysis results the use of rq=pec/pnec to evaluate the risk entropy of Shandong vegetable, vegetable farms in Fujian of Dongguan, the surrounding soil ciprofloxacin showed high risk, should focus on monitoring. Shandong Dongguan vegetable, vegetable norfloxacin enrofloxacin for moderate risk, low risk. (3) in the transmission process, a comprehensive analysis of the resistance gene, gene degradation and resistance of bacteria the degree of resistance on the basis of "gradual accumulation catastrophe" theory, establish a risk assessment system. The resistance gene by hazard identification, exposure assessment and risk characterization of 3 steps, which exposed. The comprehensive evaluation risk is divided into 4 index were evaluated: resistance index, propagation index, pollution index, degradation index. Through each index score calculation, the weight multiplied by the sum of scores after the comprehensive risk, classification of risk, relative risk grade 1-5. (4) norfloxacin, ciprofloxacin. The adsorption kinetics in three different venues in the medium of enrofloxacin were pseudo two order kinetics equation, in which the effect of organic fertilizer, the adsorption rate of three kinds of fluoroquinolone antibiotics ciprofloxacin accelerated. Which absorbed more easily, three kinds of fluoroquinolone antibiotics and migration ability of cipnorenr. in three kinds of norfloxacin, ciprofloxacin in ground medium. Thermodynamics of adsorption of enrofloxacin in line with the Freundlich model, the difference is physical adsorption. The adsorption behavior of three kinds of medium is obvious. The soil KF value respectively: 47.4679,47.2 607,33.9860; soil and fecal KF values were: 81.4329,90.1779,46.2594; soil organic fertilizer + KF = 128.0855133.5365,64.0914. (5) by soil column leaching experiment, on the 40 day test time, soil column leaching and no antibiotics, three kinds of different initial concentrations of antibiotics pollution solution in the soil column leaching was no effects of three kinds of Fluoroquinolone antibiotics leaching behavior similar. Because of norfloxacin, ciprofloxacin, enrofloxacin adsorption coefficient, soil viscosity, a part of the antibiotics adsorption by soil, three kinds of antibiotics has a short half-life, a part of its degradation, due to the presence of microorganisms in the soil environment, do not rule out by microbial degradation the possibility of soil column experiment results show that when the direct discharge of untreated antibiotics into the soil, will accumulate in the soil in a short period of time, due to the antibiotics themselves The hydrolysis effects and combined with the soil, will not cause the pollution of groundwater, but long time low dose exposure can induce the soil resistance gene, resulting in the formation of resistant bacteria, when the resistance gene in communication between different kinds of microorganisms by horizontal diffusion effects induced by super bacteria. So we must prevent antibiotics into the soil the environment. (6) by sawdust, rice husk, rice carbon, granular activated carbon, adsorption experiments showed that the activated carbon of norfloxacin, ciprofloxacin and enrofloxacin had the best effect on adsorption, the removal rate reached more than 90%. The adsorption of three kinds of fluoroquinolones with quasi two stage activated carbon adsorption kinetics, the reaction time is about 60min. Three kinds of fluoroquinolones reached equilibrium, in which the unit of activated carbon on the adsorption equilibrium of the largest amount of enrofloxacin, can reach 2000mg to three /kg; activated carbon Adsorption of fluoroquinolones with Freundlich adsorption model belongs to physical adsorption process, the KF values were 1148.9735 and 1115.8351 of norfloxacin, ciprofloxacin and enrofloxacin 1200.3835. by ultrasound showed that the activated carbon regeneration experiment in ultrasound at 25 min ultrasonic regeneration efficiency reaches the maximum, norfloxacin, ciprofloxacin and enrofloxacin were 68.5%, 68%, 69.9%; when the temperature is 35 DEG C when ultrasonic regeneration of activated carbon regeneration efficiency, norfloxacin, ciprofloxacin and enrofloxacin were 73.1%, 72.7%, 73.6%; when the ultrasonic frequency is 40 KHz, ultrasonic on activated carbon regeneration efficiency highest, norfloxacin, ciprofloxacin and enrofloxacin were 76.5%, 75.4%, 79.0%.

【學位授予單位】：東華大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：X713;X82

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