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鐵錳對(duì)Pseudomonas putida降解單苯環(huán)非甾體抗炎藥的影響

發(fā)布時(shí)間:2018-08-01 10:36
【摘要】:環(huán)境中殘留的對(duì)乙酰氨基酚(Acetaminophen,APAP)、水楊酸(Salicylic acid,SA)較難降解,污染環(huán)境且對(duì)水生動(dòng)植物有毒性作用。惡臭假單胞菌(Pseudomonas putida)廣泛存在于自然水體中,本文探討了其通過氧化鐵錳離子生成生物鐵錳氧化物降解APAP與SA這兩種單苯環(huán)非甾體抗炎藥的可行性。研究了10-500 mg/L APAP的降解可行性,10 mg/L APAP可完全降解,隨著APAP濃度增加去除率逐漸下降至零。后續(xù)主要研究10 mg/L APAP的降解特性。探究了APAP的降解條件,發(fā)現(xiàn)無鐵錳時(shí)APAP不能被降解,僅有鐵時(shí)APAP降解效果較差,鐵錳共存時(shí)降解效果最好,且錳對(duì)APAP的降解作用更大。探究了APAP降解過程中Mn~(2+)的變化規(guī)律,發(fā)現(xiàn)APAP的降解速率和Mn~(2+)的氧化速率呈強(qiáng)烈正相關(guān)。Mn~(2+)為8.13 mg/L時(shí)APAP即可完全降解,此濃度后Mn~(2+)濃度越高APAP降解速度越慢,說明過量的Mn~(2+)對(duì)細(xì)菌有毒害作用。探究了APAP降解影響因素,發(fā)現(xiàn)細(xì)菌活性受到抑制時(shí)APAP降解率降至30%,其抑制產(chǎn)物中含有9.3 mg/L Mn~(2+),而細(xì)菌活性未被抑制的Mn~(2+)為0.5 mg/L,說明細(xì)菌活性可以通過抑制Mn~(2+)氧化進(jìn)而影響APAP降解。研究了由不同濃度Mn~(2+)作用生成的不同量生物錳氧化物降解APAP的效果,發(fā)現(xiàn)生物錳氧化物量越多,APAP降解速度越快。解吸實(shí)驗(yàn)證明生物鐵錳氧化物對(duì)APAP是降解作用而非吸附作用。通過測(cè)定降解過程中總有機(jī)碳的含量,發(fā)現(xiàn)其對(duì)APAP有一定的礦化度,TOC去除率達(dá)到48.05%。上述研究證實(shí)APAP的降解主要在Pseudomonas putida氧化溶解性鐵錳離子為不溶態(tài)的生物鐵錳氧化物這一過程中的。研究了0.5-10 mg/L SA的降解可行性,發(fā)現(xiàn)SA去除率隨濃度增加而減少,0.5、1mg/L的SA可完全降解,5、10 mg/L的SA去除率分別為74.87%、61.98%。后續(xù)實(shí)驗(yàn)選取1 mg/L SA作為研究對(duì)象。探究了SA降解條件,發(fā)現(xiàn)無鐵錳時(shí)SA不能被降解,僅有鐵時(shí)SA去除率不足8%,說明鐵對(duì)降解SA所起的作用較小。探究了SA濃度對(duì)Fe~(2+)及Mn~(2+)氧化的影響,SA為1、5、10 mg/L時(shí)Fe~(2+)在1 d的氧化率分別為98.15%、96.75%、23.33%,Mn~(2+)的氧化率分別為99.59%、98.82%、44.48%,說明高濃度的SA會(huì)抑制Fe~(2+)及Mn~(2+)的氧化速度。探究了SA降解影響因素,發(fā)現(xiàn)降解效果受到細(xì)菌活性、生物鐵錳氧化物含量的影響,生物鐵錳氧化物量越多,SA去除率越高。通過解析實(shí)驗(yàn)證明生物鐵錳氧化物對(duì)SA是降解作用而非吸附作用。通過比較兩種藥物在降解過程中的差異性,發(fā)現(xiàn)APAP比SA更容易被生物鐵錳氧化物降解,去除率較高且降解所需時(shí)間較短,可被降解的濃度限值較大。相較于APAP,SA存在的環(huán)境中Pseudomonas putida氧化溶解性鐵錳離子的速度較慢。生物鐵氧化物可降解部分APAP,而對(duì)SA的降解效果非常差。降解APAP所需生物鐵錳氧化物的量較少,而SA的降解需要大量生物鐵錳氧化物來維持,尤其需要大量的生物錳氧化物。
[Abstract]:The residues of acetaminophenol (AP) and salicylic acid (SA) in the environment are difficult to degrade, which pollute the environment and have toxicity to aquatic animals and plants. Pseudomonas malodor (Pseudomonas putida) is widely found in natural water. The feasibility of degrading APAP and SA, two monobenzene nonsteroidal anti-inflammatory drugs, by ferromanganese oxide (FeMn) ion was studied. The feasibility of degradation of 10-500 mg/L APAP was studied. The degradation rate of 10-500 mg/L APAP was reduced to zero with the increase of APAP concentration for 10 mg/L APAP. The degradation characteristics of 10 mg/L APAP were studied. The degradation conditions of APAP were investigated. It was found that APAP could not be degraded without iron and manganese, but the degradation effect of APAP was poor when iron was the only one. The degradation effect of APAP was the best when iron and manganese co-existed, and the degradation effect of mn on APAP was greater than that of mn. The changes of mn ~ (2) in the degradation of APAP were studied. It was found that the degradation rate of APAP and the oxidation rate of mn ~ (2) were positively correlated with the oxidation rate of mn ~ (2). When MNO ~ (2) was 8.13 mg/L, APAP could be completely degraded, and the higher the concentration of mn ~ (2) was, the slower the degradation rate of APAP was. It shows that excessive Mn2 has toxic effect on bacteria. The factors influencing the degradation of APAP were investigated. It was found that when the bacterial activity was inhibited, the degradation rate of APAP decreased to 30%, and the inhibiting product contained 9.3 mg/L Mn2, while the uninhibited Mn2 was 0.5 mg / L, which indicated that the bacteriological activity could affect the degradation of APAP by inhibiting Mn2 oxidation. The degradation of APAP by different amounts of biological manganese oxides with different concentrations of Mn2 was studied. It was found that the more the amount of mn oxides, the faster the degradation rate of APAP was. The desorption experiment showed that the biodegradation of APAP by biological ferromanganese oxides was not adsorption. By measuring the content of total organic carbon in the degradation process, it was found that it had a certain degree of mineralization and the removal rate of APAP reached 48.05%. These results indicate that the degradation of APAP is mainly due to the fact that the oxidized dissolved iron and manganese ions of Pseudomonas putida are insoluble biological ferromanganese oxides. The feasibility of SA degradation of 0.5-10 mg/L was studied. It was found that the removal rate of SA decreased by 0.5 mg / L of SA with the increase of concentration. The total removal rate of SA for 10 mg/L was 74.87% and 61.98%, respectively. 1 mg/L SA was selected as the research object in the follow-up experiment. It was found that SA could not be degraded without iron and manganese, but the removal rate of SA was less than 8 when iron was the only one, which indicated that iron had little effect on the degradation of SA. The effect of SA concentration on the oxidation of Fe ~ (2) and mn ~ (2) was investigated. The oxidation rate of Fe ~ (2) was 98.15 ~ (5) and 96.75 ~ (53) ~ (23) mn ~ (2) at one day when SA was 1 ~ 5 ~ 5 ~ 10 mg/L, respectively. The oxidation rates of Fe ~ (2) and mn ~ (2) were 99.59 ~ (2) and 98.82 ~ (2), respectively, indicating that high concentration of SA could inhibit the oxidation rate of Fe ~ (2) and mn ~ (2). The influencing factors of SA degradation were investigated. It was found that the degradation effect was affected by the activity of bacteria and the content of biological ferromanganese oxides, and the higher the amount of biological ferromanganese oxides was, the higher the removal rate of SA was. It is proved by analytical experiments that the degradation of SA by biological ferromanganese oxides is not adsorption. By comparing the differences between the two drugs in the process of degradation, it was found that APAP was more easily degraded by biological ferromanganese oxides than SA, the removal rate was higher, the time required for degradation was shorter, and the concentration limit for degradation was higher. The oxidation rate of iron and manganese ions in the presence of Pseudomonas putida was slower than that in the presence of Pseudomonas putida SA. Biological iron oxides can degrade part of APAPs, but the degradation effect of SA is very poor. The amount of biological ferromanganese oxides needed to degrade APAP is relatively small, but the degradation of SA requires a large number of biological ferromanganese oxides to maintain, especially a large number of biological manganese oxides.
【學(xué)位授予單位】:天津理工大學(xué)
【學(xué)位級(jí)別】:碩士
【學(xué)位授予年份】:2017
【分類號(hào)】:X703

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