中間產(chǎn)物在磺胺嘧啶生物降解中的作用
發(fā)布時間：2019-05-21 21:19
【摘要】：抗生素是世界上用量最大,使用最廣泛的藥物之一,歐洲每年抗生素的使用量高達1400多噸,其中大部分用于動物;美國每年抗生素的用量約為17800噸,約70%用于畜牧水產(chǎn)養(yǎng)殖業(yè);全球抗生素年均使用總量約為100000噸~200000噸。近幾年我國每年也有成千上萬噸的抗生素類藥物被用于畜禽養(yǎng)殖業(yè)和人的醫(yī)療中,我國藥物處方中抗生素高達70%,與西方國家相對比,我國抗生素濫用情況嚴重。本實驗所研究的磺胺嘧啶(Sulfadiazine,SD),作為一種重要的抗生素類藥物,是臨床治療,畜牧業(yè)和水產(chǎn)養(yǎng)殖業(yè)中的常用抗菌藥物,由嘧啶環(huán)和苯環(huán)構(gòu)成。是一種含氮、硫的雜環(huán)化合物,是磺胺類藥物的代表,屬于較難生物降解的化合物。其進入環(huán)境后由于誘導(dǎo)耐藥菌株的產(chǎn)生而不易生物降解。然而近幾年,每年都有大量磺胺嘧啶進入環(huán)境系統(tǒng)中,可能長期存留,藥物殘留對生態(tài)系統(tǒng)和人類健康都造成危害,對磺胺類廢水的降解研究日益受到重視。目前大多數(shù)城市生活污水處理廠均以活性污泥法為主。目前,其主要功能以去除氨氮、TP、COD或BOD為主,缺乏對藥物活性組分有效去除的功能。因此,一旦污水處理系統(tǒng)遭遇到類似嘧啶藥物組分這類具有對微生物強抑制性成分的排入,輕者導(dǎo)致污水處理效率的下降,重者則導(dǎo)致整個活性污泥系統(tǒng)的崩潰。而采用有效的處理方法緩解磺胺嘧啶藥物對微生物的抑制性,加速其在環(huán)境水體中的降解速度,以避免對人類自身產(chǎn)生危害具有重要的實際意義。目前的研究發(fā)現(xiàn),針對磺胺類藥物廢水,化學(xué)氧化法處理效率較高,但降解不徹底,還可能生成對環(huán)境有不利影響的中間產(chǎn)物。而單一的生物法降解效率低,還往往受到生物抑制導(dǎo)致生物活性下降。而通過紫外光解或光催化方法作為生物方法的預(yù)處理,可以明顯地提高磺胺藥物可生化性,并提高它們的降解速率。本實驗借助紫外光解法先對SD進行降解,將降解后的SD與葡萄糖的混合溶液作為微生物生長的C、N源,探討光解處理后是否能達到緩解SD對微生物的抑制能力。同時,在紫外法加速降解磺胺嘧啶的過程中,分析紫外光照射下的中間產(chǎn)物的生成,在探究SD的光解途經(jīng)的同時,尤其是在生物降解過程中以中間產(chǎn)物作為內(nèi)援電子供體,分別采用單獨光解、單獨生物降解以及光解與生物降解同步耦合的方法對不同濃度的磺胺嘧啶和中間產(chǎn)物進行降解實驗,了解其降解規(guī)律以及礦化程度。并發(fā)現(xiàn)兩種主要中間產(chǎn)物對SD的生物降解有著一定規(guī)律的抑制或促進作用。結(jié)果表明:(1)通過紫外光照(光照強度設(shè)定為0.9mW/cm2)初始濃度為20mg/l的磺胺嘧啶(SD),在SD本身進行降解的同時,有兩種重要的中間產(chǎn)物生成,分別為對氨基苯磺酸(4-ABS)和二氨基嘧啶(2-AP),且在整個生物降解過程中可以發(fā)現(xiàn),對氨基苯磺酸的生成趨勢呈波動狀,即在初期為增長的趨勢,后期呈下降趨勢。二氨基嘧啶則呈現(xiàn)緩慢的低濃度的上升趨勢。在磺胺嘧啶(SD)降解的同時,其本身自帶的兩種離子N離子和S離子也會隨之脫離。和實驗之前推測的結(jié)果相同,N離子以銨根的形式脫除,與此同時S離子也以硫酸根的形式脫除。(2)經(jīng)過紫外光解后的磺胺嘧啶,生成的中間產(chǎn)物在接下來的生物降解過程中對磺胺嘧啶的生物降解起到了促進降解的作用。通過辯證分析實驗,將兩種中間產(chǎn)物分別與磺胺嘧啶溶液進行混合后生物降解,從結(jié)果可以證明之前的推測,即其中一種主要中間產(chǎn)物二氨基嘧啶在磺胺嘧啶生物降解中產(chǎn)生了抑制的作用,反之,另一種主要中間產(chǎn)物對氨基苯磺酸在磺胺嘧啶生物降解中有著明顯的促進作用。也同時證明了,在紫外光照后進行生物反應(yīng)的實驗中,紫外光照產(chǎn)物對氨基苯磺酸是使磺胺嘧啶降解速率明顯增加的主要原因。(3)通過提高電子數(shù)量可以將磺胺嘧啶的生物降解速率大大提高。當(dāng)所提供的電子當(dāng)量想同時,相對應(yīng)的磺胺嘧啶的降解速率也相同。通過反應(yīng)期間關(guān)于離子變化的測量與分析,可以看出,對氨基苯磺酸在生物降解的過程中并沒有釋放出S離子,但是卻在紫外光解后生物降解磺胺嘧啶的過程中促進了磺胺嘧啶脫硫的速率,使磺胺嘧啶更早的釋放出了S離子。而磺胺嘧啶經(jīng)過紫外光照后生成的兩種主要中間產(chǎn)物在其生物降解過程中分別起到了促進和抑制的作用。兩種中間產(chǎn)物之間也存在著一定的電子競爭關(guān)系。實驗結(jié)果也可以說明,磺胺嘧啶的生物降解過程中,有效電子起到了作用,但與有效電子的種類無關(guān)。綜上所述,在紫外光照后磺胺嘧啶的生物降解過程中,產(chǎn)生的中間產(chǎn)物二氨基嘧啶也同時進行生物降解,在此過程中與磺胺嘧啶產(chǎn)生了電子競爭關(guān)系,利用生成的另一種中間產(chǎn)物對氨基苯磺酸所提供的電子搶先降解,這也證實了二氨基嘧啶抑制磺胺嘧啶降解的原因。
[Abstract]:Antibiotics are the world's largest and one of the most widely used drugs, and the amount of antibiotics used in Europe is as high as 1400 tons per year, most of which are used in animals; the amount of antibiotics per year in the United States is about 17800 tons and about 70 per cent is used for livestock and aquaculture; The annual average annual use of the global antibiotics is about 100,000 tons to 200,000 tons. In recent years, in our country, thousands of tons of antibiotics are used in the livestock and poultry breeding industry and people's medical treatment. The antibiotics in our country's drug prescription are as high as 70%, compared with the western countries, the abuse of antibiotics in our country is serious. Sulfaadiazine (SD), a kind of important antibiotic medicine, is one of the most important antibiotics in clinical treatment, animal husbandry and aquaculture. Is a heterocyclic compound containing nitrogen and sulfur, and is a compound of sulfanilamide, and belongs to a compound which is difficult to be biodegraded. Which is not easy to be biodegraded due to the production of the induced drug resistant strain after entering the environment. However, in recent years, a large amount of sulfanilamide in the environmental system may remain in the environment for a long time, and the drug residue may be harmful to the ecosystem and human health, and the research on the degradation of the sulfonamides wastewater is becoming more and more important. At present, most of the urban domestic sewage treatment plants are mainly activated sludge process. At present, the main function of the invention is to remove ammonia nitrogen, TP, COD or BOD, and has the function of effectively removing the active components of the medicine. Thus, as soon as the wastewater treatment system encounters a similar fluorocarbon component of this type having a strong inhibitory component to the microorganism, the lighter results in a decrease in the efficiency of the sewage treatment, and the heavy person results in a collapse of the whole activated sludge system. And the effective treatment method is adopted to relieve the inhibitory effect of the sulfanilamide on the micro-organisms and to accelerate the degradation speed of the sulfanilamide to the environment water body so as to avoid the important practical significance to the human self-production hazard. The present study found that for sulfonamides wastewater, the treatment efficiency of the chemical oxidation process is high, but the degradation is not complete, and the intermediate products which have adverse effects on the environment can also be generated. And a single biological method is low in degradation efficiency, and is often subjected to biological inhibition, resulting in a decrease in biological activity. And the degradation rate of the sulfanilamide can be improved obviously by the pretreatment of the biological method by the ultraviolet light solution or the photocatalytic method. In this experiment, SD was first degraded by UV, and the mixed solution of SD and glucose was used as the C and N source of microbial growth. at the same time, in the process of accelerating the degradation of the sulfanilamide by the ultraviolet method, the generation of the intermediate product under the irradiation of the ultraviolet light is analyzed, The degradation experiments of sulfanilamide and intermediate products with different concentrations were carried out by the method of biodegradation and the simultaneous coupling of photolysis and biodegradation, and the degradation and the degree of mineralization were studied. It was found that the two major intermediate products could inhibit or promote the biodegradation of SD. The results showed that: (1) The initial concentration of sulfanilamide (SD) with the initial concentration of 20 mg/ l was set to be 20 mg/ l by UV irradiation (light intensity was set to 0.9 mW/ cm2), and two important intermediate products were produced in SD itself, which were p-aminobenzenesulfonic acid (4-ABS) and diamino-benzenesulfonic acid (2-AP), respectively. And during the whole biodegradation process, the production trend of the p-aminobenzenesulfonic acid is in a wave shape, that is, the trend of the growth in the early stage is the trend of the growth, and the later period is in a downward trend. The diaminopterin presents a slow, low concentration of the upward trend. At the same time of the degradation of the sulfanilamide (SD), the ion and the S-ion of the two ions are also separated from each other. And the S-ions are also removed in the form of sulfate. (2) the prepared intermediate product has the effect of promoting the degradation of the sulfanilamide peroxide in the subsequent biodegradation process through the sulfanilamide peroxide solution after the ultraviolet light solution. According to the dialectical analysis experiment, the two intermediate products are respectively mixed with the sulfanilamide peroxide solution to be biodegraded, and the result can be proved that one of the main intermediate products, the diaminopterin, has the effect of inhibition in the biodegradation of the sulfanilamide, and vice versa, The other major intermediate product has a significant effect on the biodegradation of the sulfanilamide in the sulfanilamide. It is also proved that in the experiments of the biological reaction after the ultraviolet irradiation, the UV-light product is the main cause of the apparent increase of the degradation rate of the sulfanilamide. (3) The rate of biodegradation of the sulfanilamide peroxide can be greatly improved by increasing the number of electrons. The rate of degradation of the corresponding sulfanilamide is also the same when the supplied electron equivalent is desired. Through the measurement and analysis of the ion change during the reaction, it can be seen that the p-aminobenzenesulfonic acid does not release the S ions in the process of biodegradation, but the rate of the sulfanilamide peroxide desulfurization is promoted in the process of degrading the sulfanilamide peroxide after the ultraviolet light is released, And the sulfanilamide is released to release the S ions earlier. In the process of biodegradation, the two main intermediates produced by the ultraviolet irradiation of the sulfanilamide have the effects of promoting and inhibiting. There is also a certain electronic competitive relationship between the two intermediate products. The experimental results also show that the effective electrons play an important role in the process of biodegradation of sulfanilamide, but not related to the species of active electrons. In conclusion, in the process of the biodegradation of the sulfanilamide peroxide after the ultraviolet irradiation, the intermediate product diaminopterin is also biodegraded at the same time, and the electronic competitive relationship with the sulfanilamide peroxide is generated in the process, The use of the resulting further intermediate product for the pre-emptive degradation of the p-aminobenzenesulfonic acid also confirmed the reason for the diamino-benzenesulfonic acid to inhibit the degradation of the sulfanilamide.
【學(xué)位授予單位】：上海師范大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：X703
本文編號：2482406
[Abstract]:Antibiotics are the world's largest and one of the most widely used drugs, and the amount of antibiotics used in Europe is as high as 1400 tons per year, most of which are used in animals; the amount of antibiotics per year in the United States is about 17800 tons and about 70 per cent is used for livestock and aquaculture; The annual average annual use of the global antibiotics is about 100,000 tons to 200,000 tons. In recent years, in our country, thousands of tons of antibiotics are used in the livestock and poultry breeding industry and people's medical treatment. The antibiotics in our country's drug prescription are as high as 70%, compared with the western countries, the abuse of antibiotics in our country is serious. Sulfaadiazine (SD), a kind of important antibiotic medicine, is one of the most important antibiotics in clinical treatment, animal husbandry and aquaculture. Is a heterocyclic compound containing nitrogen and sulfur, and is a compound of sulfanilamide, and belongs to a compound which is difficult to be biodegraded. Which is not easy to be biodegraded due to the production of the induced drug resistant strain after entering the environment. However, in recent years, a large amount of sulfanilamide in the environmental system may remain in the environment for a long time, and the drug residue may be harmful to the ecosystem and human health, and the research on the degradation of the sulfonamides wastewater is becoming more and more important. At present, most of the urban domestic sewage treatment plants are mainly activated sludge process. At present, the main function of the invention is to remove ammonia nitrogen, TP, COD or BOD, and has the function of effectively removing the active components of the medicine. Thus, as soon as the wastewater treatment system encounters a similar fluorocarbon component of this type having a strong inhibitory component to the microorganism, the lighter results in a decrease in the efficiency of the sewage treatment, and the heavy person results in a collapse of the whole activated sludge system. And the effective treatment method is adopted to relieve the inhibitory effect of the sulfanilamide on the micro-organisms and to accelerate the degradation speed of the sulfanilamide to the environment water body so as to avoid the important practical significance to the human self-production hazard. The present study found that for sulfonamides wastewater, the treatment efficiency of the chemical oxidation process is high, but the degradation is not complete, and the intermediate products which have adverse effects on the environment can also be generated. And a single biological method is low in degradation efficiency, and is often subjected to biological inhibition, resulting in a decrease in biological activity. And the degradation rate of the sulfanilamide can be improved obviously by the pretreatment of the biological method by the ultraviolet light solution or the photocatalytic method. In this experiment, SD was first degraded by UV, and the mixed solution of SD and glucose was used as the C and N source of microbial growth. at the same time, in the process of accelerating the degradation of the sulfanilamide by the ultraviolet method, the generation of the intermediate product under the irradiation of the ultraviolet light is analyzed, The degradation experiments of sulfanilamide and intermediate products with different concentrations were carried out by the method of biodegradation and the simultaneous coupling of photolysis and biodegradation, and the degradation and the degree of mineralization were studied. It was found that the two major intermediate products could inhibit or promote the biodegradation of SD. The results showed that: (1) The initial concentration of sulfanilamide (SD) with the initial concentration of 20 mg/ l was set to be 20 mg/ l by UV irradiation (light intensity was set to 0.9 mW/ cm2), and two important intermediate products were produced in SD itself, which were p-aminobenzenesulfonic acid (4-ABS) and diamino-benzenesulfonic acid (2-AP), respectively. And during the whole biodegradation process, the production trend of the p-aminobenzenesulfonic acid is in a wave shape, that is, the trend of the growth in the early stage is the trend of the growth, and the later period is in a downward trend. The diaminopterin presents a slow, low concentration of the upward trend. At the same time of the degradation of the sulfanilamide (SD), the ion and the S-ion of the two ions are also separated from each other. And the S-ions are also removed in the form of sulfate. (2) the prepared intermediate product has the effect of promoting the degradation of the sulfanilamide peroxide in the subsequent biodegradation process through the sulfanilamide peroxide solution after the ultraviolet light solution. According to the dialectical analysis experiment, the two intermediate products are respectively mixed with the sulfanilamide peroxide solution to be biodegraded, and the result can be proved that one of the main intermediate products, the diaminopterin, has the effect of inhibition in the biodegradation of the sulfanilamide, and vice versa, The other major intermediate product has a significant effect on the biodegradation of the sulfanilamide in the sulfanilamide. It is also proved that in the experiments of the biological reaction after the ultraviolet irradiation, the UV-light product is the main cause of the apparent increase of the degradation rate of the sulfanilamide. (3) The rate of biodegradation of the sulfanilamide peroxide can be greatly improved by increasing the number of electrons. The rate of degradation of the corresponding sulfanilamide is also the same when the supplied electron equivalent is desired. Through the measurement and analysis of the ion change during the reaction, it can be seen that the p-aminobenzenesulfonic acid does not release the S ions in the process of biodegradation, but the rate of the sulfanilamide peroxide desulfurization is promoted in the process of degrading the sulfanilamide peroxide after the ultraviolet light is released, And the sulfanilamide is released to release the S ions earlier. In the process of biodegradation, the two main intermediates produced by the ultraviolet irradiation of the sulfanilamide have the effects of promoting and inhibiting. There is also a certain electronic competitive relationship between the two intermediate products. The experimental results also show that the effective electrons play an important role in the process of biodegradation of sulfanilamide, but not related to the species of active electrons. In conclusion, in the process of the biodegradation of the sulfanilamide peroxide after the ultraviolet irradiation, the intermediate product diaminopterin is also biodegraded at the same time, and the electronic competitive relationship with the sulfanilamide peroxide is generated in the process, The use of the resulting further intermediate product for the pre-emptive degradation of the p-aminobenzenesulfonic acid also confirmed the reason for the diamino-benzenesulfonic acid to inhibit the degradation of the sulfanilamide.
【學(xué)位授予單位】：上海師范大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：X703
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