本文關(guān)鍵詞： 藥品及個(gè)人護(hù)理用品 高級(jí)氧化 消毒副產(chǎn)物 影響因素　出處：《江西理工大學(xué)》2015年碩士論文　論文類型：學(xué)位論文

【摘要】：典型的新型污染物之一——藥品及個(gè)人護(hù)理用品(Pharmaceuticals and Personal Care Products,PPCPs)在環(huán)境中的普遍存在使其正以潛移默化的方式影響著生態(tài)環(huán)境與動(dòng)植物健康。而飲用水消毒工藝在與病原微生物反應(yīng)的同時(shí)也會(huì)與原水中有機(jī)物互相反應(yīng)生成高“三致”風(fēng)險(xiǎn)物質(zhì)——消毒副產(chǎn)物(Disinfection By-products,DBPs),當(dāng)PPCPs作為其前體物時(shí),生成的DBPs相較于其本身毒性將大幅度提高。本課題利用UV/PS(Persulfate,PS)與UV/H2O2兩種高級(jí)氧化工藝對(duì)比、陰離子活化PMS(Peroxymonosulfate,PMS)降解水中磺胺類藥物增效劑甲氧芐氨嘧啶(Trimethoprim,TMP),采用Fe2+/UV活化PMS去除水中抗癲癇藥物卡馬西平(Carbamazepine,CBZ)。著重討論氧化劑濃度、目標(biāo)污染物濃度、催化劑濃度、p H值、腐殖酸(Humic Acid,HA)與陰離子濃度等影響因素對(duì)相應(yīng)高級(jí)氧化方法去除PPCPs的影響并分析其反應(yīng)機(jī)理。以CBZ和TMP,并增設(shè)金霉素(Chlorotetracycline,CTC)為前體物,對(duì)比并歸納自由氯消毒與氯胺消毒兩種方式的DBPs生成規(guī)律,最后考察UV/PS、UV/H2O2和Fe2+/UV/PMS三種高級(jí)氧化前處理對(duì)PPCPs的DBPs生成影響。研究表明:(1)UV/PS、UV/H2O2兩種方法對(duì)TMP的降解都符合偽一級(jí)動(dòng)力學(xué)模型,在室溫條件下,前者對(duì)TMP的去除率略高于后者。堿性反應(yīng)條件不利于TMP的去除;共存陰離子對(duì)反應(yīng)的影響作用十分復(fù)雜,其中,CO32-與HCO3-始終表現(xiàn)出對(duì)反應(yīng)的抑制作用。(2)五種陰離子(CO32-、Cl-、HPO42-、NO3-、SO42-)中,NO3-和SO42-對(duì)PMS基本無(wú)活化能力;CO32-、Cl-和HPO42-三種離子活化PMS所產(chǎn)生的強(qiáng)氧化性活性物種分別為HCO4-、HOCl和SO4-·;當(dāng)反應(yīng)p H值升至一定程度時(shí),TMP的去除主要是PMS的堿活化作用的結(jié)果;不同于其它高級(jí)氧化方法,HA不會(huì)對(duì)陰離子活化PMS反應(yīng)產(chǎn)生顯著影響。(3)通過(guò)Fe2+/UV活化PMS法對(duì)水中CBZ進(jìn)行降解時(shí)發(fā)現(xiàn),過(guò)高的氧化劑與催化劑濃度、減小UV輻照面積、增高反應(yīng)p H值和增高HA濃度皆不利于降解反應(yīng)的進(jìn)行;提高CBZ的去除率可通過(guò)分次投加Fe2+和加入適量檸檬酸鹽兩種方法實(shí)現(xiàn)。(4)CBZ、TMP和CTC在氯化后生成了大量的DBPs,其生成量與前體物分子中碳原子數(shù)量、培養(yǎng)時(shí)間和加氯量成正比,也與前體物本身性質(zhì)有關(guān);培養(yǎng)過(guò)程中會(huì)出現(xiàn)不同種類DBPs間的相互轉(zhuǎn)化現(xiàn)象,長(zhǎng)時(shí)間的培養(yǎng)也會(huì)使部分DBPs自身?yè)]發(fā)與分解;氯胺消毒能顯著控制含碳消毒副產(chǎn)物(C-DBPs)的產(chǎn)量;在所能檢測(cè)的DBPs中,均表現(xiàn)出在中性條件下生成濃度達(dá)到最大的規(guī)律。(5)使用高級(jí)氧化前處理方法能夠大量去除被檢出DBPs的前體物,并改變其結(jié)構(gòu),使其難以再被氯化,從而達(dá)到抑制DBPs生成的目的。
[Abstract]:One of the typical new pollutants, and Personal Care products (PPCPs), is affecting the ecological environment and animal and plant health in an imperceptible way because of its widespread presence in the environment. At the same time, the protozoa react with organic matter in raw water to form a high "three cause" risk substance, disinfection By-productsDBPsN, when PPCPs is used as its precursor. The DBPs produced will be much more toxic than its own toxicity. In this study, two advanced oxidation processes, UV / PS / sulfatePSand UV/H2O2, were used to compare the two advanced oxidation processes. Anion activated PMS-PeroxymonosulfatePMSs were used to degrade trimethoprimidine trimethoprimidine trimethoprimidine (trimethoprimidine) in water, and Fe2 / UV activated PMS was used to remove carbamazepine. The concentration of oxidant, the concentration of target pollutants and the concentration of catalyst were discussed. Humic acid acid acid (Humic acid acid) and anion concentration influence the removal of PPCPs by the advanced oxidation method and analyze its reaction mechanism. CBZ and TMP were used as precursors, and chlortetracycline CTC was added as the precursor. The rules of DBPs formation in two ways of free chlorine disinfection and chloramine disinfection were compared and summarized. Finally, the effects of three advanced oxidation pretreatments on the DBPs production of PPCPs were investigated. The results showed that the degradation of TMP by the two methods was in accordance with the pseudo-first-order kinetic model at room temperature. The removal rate of TMP in the former is slightly higher than that in the latter. The basic reaction conditions are not conducive to the removal of TMP, and the influence of coexisting anions on the reaction is very complex. The five anions (CO32-Cl-HPO42-HPO42-NO3-O4-SO42-) and so _ 42- have little ability to activate PMS. The strong oxidizing active species produced by the activation of PMS by the three kinds of ions are HCO4-HHOCl and SO4- 路, respectively, when the reaction p, the active species are HCO4-HHOCl and SO4-, respectively, when the reaction p, the active species of PMS are HCO4-OHCl and SO4- 路, respectively, when the reaction p, the active species are HCO4-HHOCl and so _ 4- 路. When H value rises to a certain extent, the removal of TMP is mainly the result of alkali activation of PMS. Different from other advanced oxidation methods, the anion activated PMS reaction was not significantly affected by HA. (3) when CBZ in water was degraded by Fe2 / UV activated PMS method, it was found that the excessive concentration of oxidant and catalyst reduced the irradiation area of UV. Increasing the pH value of the reaction and increasing the concentration of HA were not conducive to the degradation reaction. Increasing the removal rate of CBZ can be achieved by adding Fe2 and adding appropriate amount of citrate to produce a large amount of DBPs after chlorination, which is directly proportional to the amount of carbon atoms in the precursor molecule, the culture time and the amount of chlorine added. It also has something to do with the properties of precursors, the mutual transformation of different kinds of DBPs will occur in the culture process, the long time culture will also make part of DBPs volatilize and decompose, chloramine disinfection can significantly control the yield of carbon-containing disinfection by-products (C-DBPss). In the DBPs that can be detected, it is shown that the formation concentration reaches the maximum rule under neutral conditions. 5) the advanced oxidation pretreatment method can remove the precursors of the detected DBPs and change its structure so that it is difficult to chlorinate. In order to achieve the purpose of inhibiting the formation of DBPs.
【學(xué)位授予單位】：江西理工大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：TU991.25

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本文編號(hào)：1499642