【摘要】：自然水體中的藥物及個(gè)人護(hù)理品(PPCPs)對(duì)人體和環(huán)境具有潛在的危害,傳統(tǒng)的廢水處理技術(shù)難以對(duì)其有效去除,如何將其有效去除成為研究焦點(diǎn)。電離輻照技術(shù)作為一種高級(jí)氧化技術(shù),在水處理領(lǐng)域日益得到重視,具有潛在的應(yīng)用前景。論文選取甲氧芐氨嘧啶、卡馬西平和三氯生為代表性PPCPs,研究了三種PPCPs輻照降解的影響因素,探討了其輻照降解動(dòng)力學(xué)特性,提出了降解路徑,考察了輻照技術(shù)與其他氧化技術(shù)聯(lián)合對(duì)PPCPs降解的作用,并比較了PPCPs輻照前后的可生化性變化。主要結(jié)論如下:(1)研究了影響PPCPs輻照降解的主要因素,包括PPCPs的初始濃度,其他氧化劑的投加量和溶液初始pH值。結(jié)果表明,較低的濃度有利于PPCPs降解與礦化。過(guò)硫酸鉀的加入對(duì)PPCPs輻照降解具有顯著的促進(jìn)作用。當(dāng)K2S2O8投加量為1.5 mM時(shí),在1000 Gy的吸收劑量下各PPCPs的礦化率由16%-34%提升至32%-94.1%。K2FeO4的加入在輻照降解初期對(duì)PPCPs的去除有抑制作用,隨后卻在一定程度上提高了礦化率。在偏酸性條件下(pH=6.5)有利于各PPCPs的輻照降解。(2)分析了不同輻照體系下PPCPs的輻照降解動(dòng)力學(xué)。結(jié)果表明三種PPCPs的在不同輻照體系中的降解符合準(zhǔn)一級(jí)動(dòng)力學(xué)反應(yīng)規(guī)律。(3)探討了各PPCPs在不同輻照體系下的降解途徑和機(jī)理。結(jié)果表明甲氧芐氨嘧啶主要通過(guò)羥基化、去甲基化、裂解以及脫氫作用實(shí)現(xiàn)降解和礦化;卡馬西平的降解主要通過(guò)羥基化和裂解作用實(shí)現(xiàn);而三氯生的降解則通過(guò)羥基化、脫氯及裂解作用實(shí)現(xiàn)。在各過(guò)程中HO·起主要作用,SO4-·通過(guò)電子傳遞促進(jìn)HO·降解PPCPs的反應(yīng)進(jìn)程,而Fe(VI)則直接氧化PPCPs實(shí)現(xiàn)對(duì)其的降解。(4)通過(guò)比較活性污泥呼吸耗氧量,考察了輻照前后PPCPs的可生化性。結(jié)果表明:各PPCPs在輻照前難以被生物利用甚至具有生物毒性,輻照處理后其可生化性提高。輻照處理含1 mg/L甲氧芐氨嘧啶/三氯生的二級(jí)出水經(jīng)過(guò)曝氣生物濾池處理后發(fā)現(xiàn)COD、TOC和NH4+-N的去除率均顯著提高。這為輻照技術(shù)與曝氣生物濾池工藝聯(lián)合應(yīng)用于二級(jí)出水深度處理提供了理論依據(jù)和技術(shù)支持。研究對(duì)輻照技術(shù)處理含PPCPs的廢水具有重要的理論和實(shí)際應(yīng)用價(jià)值。
[Abstract]:Drugs and personal care products (PPCPs) in natural water have potential harm to human body and environment. It is difficult for traditional wastewater treatment technology to remove them effectively. How to remove them effectively has become the focus of research. As a kind of advanced oxidation technology, ionizing irradiation technology has been paid more and more attention in the field of water treatment and has a potential application prospect. In this paper, trimethoprim, carbamazepine and triclosan were selected as representative PPCPs, to study the influencing factors of three kinds of PPCPs irradiation degradation. The effects of irradiation and other oxidation technologies on the degradation of PPCPs were investigated, and the biodegradability of PPCPs before and after irradiation was compared. The main conclusions are as follows: (1) the main factors affecting the degradation of PPCPs irradiated were studied, including the initial concentration of PPCPs, the dosage of other oxidants and the initial pH value of the solution. The results showed that low concentration was beneficial to PPCPs degradation and mineralization. The addition of potassium persulfate can significantly promote the degradation of PPCPs by irradiation. When the dosage of K2S2O8 was 1.5 mM, at the absorbed dose of 1000 Gy, the mineralization rate of each PPCPs increased from 16% to 34%, and the addition of 32%-94.1%.K2FeO4 inhibited the removal of PPCPs at the early stage of irradiation degradation. Subsequently, the mineralization rate was increased to a certain extent. Under the condition of partial acidity (pH=6.5), the irradiation degradation of PPCPs was facilitated. (2) the kinetics of irradiation degradation of PPCPs in different irradiation systems was analyzed. The results show that the degradation of three kinds of PPCPs in different irradiation systems accords with the quasi-first-order kinetic reaction law. (3) the degradation pathway and mechanism of PPCPs in different irradiation systems are discussed. The results showed that the degradation and mineralization of trimethoprim were mainly achieved by hydroxylation demethylation cracking and dehydrogenation while the degradation of carbamazepine was mainly achieved by hydroxylation and cleavage. The degradation of triclosan was achieved by hydroxylation, dechlorination and pyrolysis. HO plays a major role in each process. SO4- promotes the degradation of PPCPs by HO through electron transfer, while Fe (VI) directly oxidizes PPCPs to achieve its degradation. (4) oxygen consumption in respiration of activated sludge is compared. The biodegradability of PPCPs before and after irradiation was investigated. The results showed that each PPCPs was difficult to be bioutilized or even biotoxic before irradiation, and its biodegradability was improved after irradiation. The removal rates of COD,TOC and NH4-N in the secondary effluent containing 1 mg/L trimethoprim / trichlorogenate were significantly increased after biological aerated filter treatment. This provides a theoretical basis and technical support for the combined application of irradiation technology and biological aerated filter in advanced treatment of secondary effluent. The study has important theoretical and practical application value for the treatment of wastewater containing PPCPs by irradiation technology.
【學(xué)位授予單位】：中國(guó)地質(zhì)大學(xué)(北京)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2017
【分類號(hào)】：X703

【相似文獻(xiàn)】

相關(guān)期刊論文 前10條

1 張登平;王廣華;;甲氧芐氨嘧啶生產(chǎn)中"二氧化錳"污泥的回收利用[J];環(huán)境科學(xué)動(dòng)態(tài);1985年10期

2 周杰,何錫文,趙潔,史慧明;藥物甲氧芐氨嘧啶分子模板聚合物結(jié)合作用及選擇性研究[J];高等學(xué)校化學(xué)學(xué)報(bào);1999年02期

3 陳仁夫;粟淑華;賀廣達(dá);汪玉英;胡英秀;;甲氧芐氨嘧啶雜質(zhì)甲�？s胍胺的來(lái)源及其對(duì)質(zhì)量影響的研究[J];醫(yī)藥工業(yè);1980年01期

4 鄧桂勤;李勇;;高效液相色譜法測(cè)甲氧芐氨嘧啶含量[J];光譜儀器與分析;1996年03期

5 楊長(zhǎng)志;康慶賀;馬東升;韓廣源;;高效液相色譜法測(cè)定動(dòng)物源性食品中甲氧芐氨嘧啶殘留量[J];化學(xué)工程師;2005年12期

6 吳謀成;用高效液相色譜測(cè)定動(dòng)物血清中甲氧芐氨嘧啶和磺胺-5-甲氧嘧啶[J];色譜;1986年06期

7 高建華,林鵬,陳彬;熒光分光光度法直接測(cè)定炎痢停片中的甲氧芐氨嘧啶和氟哌酸[J];分析試驗(yàn)室;1999年06期

8 尚秀敏，，田蘭，郭毅;一階導(dǎo)數(shù)光譜法測(cè)定增效黃連素膠囊中甲氧芐氨嘧啶的含量[J];河北醫(yī)學(xué)院學(xué)報(bào);1995年05期

9 杜鎬;徐幗倩;黃婕;;高效液相色譜法測(cè)定甲氧芐氨嘧啶中的腈類雜質(zhì)[J];西安礦業(yè)學(xué)院學(xué)報(bào);1991年04期

10 張進(jìn)治,汪瑗;甲氧芐氨嘧啶的表面增強(qiáng)拉曼光譜研究[J];光譜學(xué)與光譜分析;2003年01期

相關(guān)重要報(bào)紙文章 前1條

1 倪文昊;實(shí)話實(shí)說(shuō)反傾銷[N];醫(yī)藥經(jīng)濟(jì)報(bào);2006年

相關(guān)博士學(xué)位論文 前1條

1 張忠磊;電離輻照聯(lián)合BAF處理水中藥物及抗菌劑的研究[D];中國(guó)地質(zhì)大學(xué)(北京);2017年

本文編號(hào)：2311685