發(fā)布時(shí)間：2017-12-27 05:16

  本文關(guān)鍵詞：城市生活垃圾填埋場(chǎng)中抗生素殘留濃度征及抗性基因相關(guān)性研究　出處：《華東師范大學(xué)》2017年碩士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： 城市垃圾填埋場(chǎng) 滲濾液 固體廢棄物 抗生素 抗性基因

【摘要】：抗生素(Antibiotics,ABs)濫用是目前許多國(guó)家和地區(qū)面臨的重要問題,其在環(huán)境中的殘留加速誘導(dǎo)了環(huán)境中耐藥性細(xì)菌以及抗生素抗性基因(Antibiotic Resistance Genes,ARGs)的產(chǎn)生、傳播,對(duì)周邊環(huán)境帶來潛在生態(tài)和健康風(fēng)險(xiǎn)。我國(guó)是抗生素生產(chǎn)和使用大國(guó),藥物因回收體制不健全,大多混入日常生活垃圾進(jìn)入城市生活垃圾填埋場(chǎng),但目前對(duì)于城市生活垃圾填埋場(chǎng)中抗生素殘留及其濃度特征的研究卻鮮有報(bào)道。關(guān)注城市生活垃圾填埋場(chǎng)環(huán)境介質(zhì)中的抗生素殘留及其抗性基因之間相關(guān)性研究,對(duì)提高關(guān)于抗生素的認(rèn)識(shí)及其風(fēng)險(xiǎn)意識(shí)具有重要意義。本研究采集了上海市老港和黎明城市生活垃圾填埋場(chǎng)固體廢棄物和滲濾液樣品,采用SAX-HLB串聯(lián)固相萃取和超高效液相色譜三重四級(jí)桿質(zhì)譜聯(lián)用儀(UPLC-3QMS)檢測(cè)分析填埋場(chǎng)固體廢棄物和滲濾液中15種抗生素的檢出濃度及其濃度分布特征;采用熒光定量PCR分析填埋場(chǎng)固體廢棄物和滲濾液中7種抗生素抗性基因。探討了填埋場(chǎng)環(huán)境中抗生素及其抗性基因之間的相關(guān)性,為城市生活垃圾填埋場(chǎng)中抗生素的遷移轉(zhuǎn)化、風(fēng)險(xiǎn)評(píng)估提供參考依據(jù)。研究發(fā)現(xiàn),在填埋場(chǎng)滲濾液中,四環(huán)素類(TCs)、喹諾酮類(FQs)、磺胺類(SAs)、大環(huán)內(nèi)脂類(MLs)、β-內(nèi)酰胺類(BLs)5類15種抗生素在滲濾液中均有不同濃度檢出,其中磺胺二甲基嘧啶(SMZ)、諾氟沙星(NOR)、氧氟沙星(OFL)、羅紅霉素(RTM)和去水紅霉素(ETM-H_2O)5種抗生素檢出率達(dá)到100%。去水紅霉素在滲濾液中檢出濃度最高(20200.0 ng/L),平均檢出濃度達(dá)到5695.7 ng/L,其次分別為OFL、NOR,最高檢出濃度分別為6950.0 ng/L、3225.0 ng/L,平均檢出濃度分別為1870.9 ng/L、1101.2 ng/L,阿莫西林在滲濾液中檢出濃度較低,平均檢出濃度僅為8.6 ng/L,檢出率22.0%�？股卦诶淆g滲濾液(3075.8±4004.0ng/L)中濃度均低于新鮮(15063.6±2475.9ng/L)和黎明滲濾液(13628.5±8792.5 ng/L)中濃度(pp0.01),老港新鮮和黎明滲濾液中抗生素檢出濃度無明顯差異(p=0.107)。三種滲濾液(老港老齡、新鮮和黎明滲濾液)在雨季的抗生素濃度相比旱季滲濾液中的濃度均存在不同程度降低,其中老齡滲濾液和黎明滲濾液中抗生素濃度下降程度分別達(dá)到93%(5737.9±4229.4 ng/L vs 413.6±38.0ng/L)和 78%(22398.6±887.1 ng/L vs 4858.4±24.4ng/L);而新鮮滲濾液中抗生素濃度僅下降28%(17135.0±1931.4 ng/L vs 13003.4±322.6 ng/L),濃度下降程度較低。在填埋場(chǎng)固體廢棄物中,TCs、QNs、MLs三類9種抗生素的檢出率均達(dá)到100%,SAs和BLs兩類抗生素的檢出率為23.4-93.6%;喹諾酮類抗生素NOR和OFL最高檢出濃度分別達(dá)到1497.5 μg/kg和1250.0 μg/kg,平均檢出濃度分別為260.1 μg/kg和215.8 μg/kg,阿莫西林(AMOX)在所有固體廢棄物樣品中的檢出濃度普遍較低,平均檢出濃度小于0.1 μg/kg。相比黎明填埋場(chǎng)固體廢棄物中的抗生素檢出濃度,TCs、QNs和MLs三類抗生素在老港填埋場(chǎng)固體廢棄物中的抗生素檢出濃度均普遍降低(p0.05),而SAs和BLs在兩個(gè)填埋場(chǎng)固體廢棄物中的檢出濃度無顯著變化。在老港填埋場(chǎng)填埋表層(0.5-1.5m)的固體廢棄物樣品中,呈現(xiàn)出抗生素濃度在深度上的變化特征,除BLs外其它四類抗生素(TCs、QNs、SAs、MLs)在1.5 m深度處的抗生素檢出濃度均高于其在0.5 m深度處的檢出濃度(p0.05),而黎明填埋場(chǎng)填埋表層固體廢棄物中則無此濃度分布特征。這可能是由于老港填埋場(chǎng)中固體廢棄物已處于填埋成熟階段,且抗生素在雨水、滲濾液等作用向下遷移擴(kuò)散所致。研究選擇檢測(cè)了 7種抗生素抗性基因(tetQ、tetW、mefA、ermB、sul1、sul2和mexF)以及整合子int1。檢測(cè)結(jié)果顯示,在填埋場(chǎng)滲濾液中,7種ARGs的檢出濃度為2.91×10~2～4.88×10~6 copies/ngDNA,整合子int1檢出濃度為4.55×10~4～8.31×10~7 copies/ngDNA;在填埋場(chǎng)固體廢棄物中,tetQ、tetM、mefA三種ARGs檢出濃度低于標(biāo)準(zhǔn)曲線定量范圍,ermB、sul1、sul2和mexF四種ARGs的檢出濃度為1.85×1 02～5.07×1 06 copies/ngDNA,整合子int1檢出濃度為6.90×105～1.86×108 copies/ngDNA。分析抗生素與其抗性基因之間相關(guān)性結(jié)果表明,在填埋場(chǎng)滲濾液中,四環(huán)素類抗生素均與抗性基因tetQ之間呈現(xiàn)顯著相關(guān)性,ETM-H_2O、MLs與mefA存在顯著相關(guān)性,磺胺甲惡唑(SMX)、SAs則與sul1和sul2呈現(xiàn)顯著負(fù)相關(guān)性,而多重抗性基因mexF與所檢測(cè)抗生素之間均無相關(guān)性;在老港填埋表層固體廢棄物中,僅RTM與ermB具有顯著正相關(guān)性,與多重抗性基因mexF呈現(xiàn)顯著負(fù)相關(guān)性;在黎明填埋場(chǎng)表層固體廢棄物中,僅sul2與磺胺嘧啶(SD)、磺胺二甲基嘧啶(SMZ)以及SAs呈現(xiàn)顯著負(fù)相關(guān)性。這可能是因?yàn)槌鞘猩罾盥駡?chǎng)環(huán)境介質(zhì)理化性質(zhì)(溫度、光照、pH等)復(fù)雜,污染物質(zhì)(重金屬、有毒物質(zhì)等)濃度高,影響ARGs在填埋場(chǎng)中的誘導(dǎo)產(chǎn)生、衰減和傳播擴(kuò)散。在滲濾液中,整合子intl與sul1、sul2和mexF之間存在極顯著正相關(guān)性,在老港填埋場(chǎng)固體廢棄物中整合子int1與sul1和sul2之間極顯著相關(guān),但其在黎明填埋場(chǎng)固體廢棄物中與ermB、sul1、sul2以及mexF均無相關(guān)性,這可能表明在固體廢棄物填埋后期,抗性基因sul1、sul2以水平基因轉(zhuǎn)移為重要途徑在固體廢棄物中的傳播擴(kuò)散。綜上所述,本研究中15種常用抗生素在城市生活垃圾填埋場(chǎng)表層固體廢棄物和滲濾液中均能高濃度檢出,且不同種類的抗生素檢出濃度之間存在差異�？剐曰蚺c部分種類的殘留抗生素之間顯著相關(guān),但填埋場(chǎng)環(huán)境介質(zhì)復(fù)雜的理化性質(zhì)和高濃度的污染物質(zhì)影響ARGs在填埋場(chǎng)中的誘導(dǎo)產(chǎn)生、衰減和傳播擴(kuò)散。
[Abstract]:The abuse of antibiotics (Antibiotics, ABs) is an important problem in many countries and regions are currently facing, the residue in the environment to accelerate the environment induced by antibiotic resistant bacteria and antibiotic resistance genes (Antibiotic, Resistance Genes, ARGs) generation, propagation, potential ecological and health risk to the surrounding environment. China is a large country in the field of antibiotic production and use. Because of the imperfect system of recovery, most of the drugs are mixed into daily life garbage to enter the municipal solid waste landfill site. However, the research on the residual and concentration characteristics of antibiotics in MSW landfill is rarely reported. Concerned about the correlation between antibiotic residues and their resistance genes in municipal solid waste landfill sites, it is of great significance to improve the awareness and risk awareness of antibiotics. This study collected in Shanghai city and the old port city dawn landfill of solid waste and leachate samples by SAX-HLB solid-phase extraction and ultra performance liquid chromatography three four quadrupole mass spectrometry (UPLC-3QMS) detection concentration and concentration distribution of 15 kinds of antibiotics in solid waste landfill and leachate detection analysis; using fluorescence quantitative PCR analysis of 7 kinds of antibiotic resistance genes and solid waste landfill leachate. The correlation between antibiotics and their resistance genes in the landfill environment is discussed, so as to provide references for the migration, transformation and risk assessment of antibiotics in municipal solid waste landfill. The study found that in the landfill leachate, tetracyclines and quinolones (TCs) (FQs) (SAs), sulfonamides, macrolides (MLs), beta lactam (BLs) 5 categories of 15 kinds of antibiotics in the leachate were detected at different concentrations, the sulfamethazine (SMZ), norfloxacin (NOR), ofloxacin (OFL), roxithromycin (RTM) and erythromycin (ETM-H_2O) water to 5 kinds of antibiotics detection rate reached 100%. Go to the water in the leachate were erythromycin the highest concentration (20200 ng/L), the average detection concentration reached 5695.7 ng/L, followed by OFL, NOR, the highest concentration were 6950 ng/L, 3225 ng/L, the average detection concentration were 1870.9 ng/L, 1101.2 ng/L, Amos Lin in the leachate were detected in low concentrations, the average detection the concentration is 8.6 ng/L, the detection rate of 22%. The concentration of antibiotics in the aged leachate (3075.8 + 4004.0ng/L) was lower than that in fresh (15063.6 + 2475.9ng/L) and leachate (13628.5 + 8792.5 ng/L) concentration (pp0.01). There was no significant difference in the concentration of antibiotics in fresh port and leachate in old port (p=0.107). Three kinds of leachate (Hong Kong, fresh and old aged dawn leachate) concentration in leachate infiltration compared to dry season there are different degrees of reduction in the concentration of antibiotics during the rainy season, the aging of leachate and leachate infiltration dawn antibiotic concentration decreased respectively 93% (5737.9 + 4229.4 ng/ L vs 413.6 + 38.0ng/L and 78% (22398.6) 887.1 + ng/L vs 4858.4 + 24.4ng/L); while the fresh leachate concentration of antibiotics decreased only 28% (17135 + 1931.4 + 322.6 ng/L vs 13003.4 ng/L), decreased the concentration of low degree. In the landfill of solid waste, TCs, QNs, MLs three categories of 9 kinds of antibiotics detection rate reached 100%, the detection of SAs and BLs two kinds of antibiotics was 23.4-93.6%; NOR and OFL highest quinolone antibiotics detection concentration reached 1497.5 g/kg and 1250 g/kg, the average detection concentration were 260.1 g/kg and 215.8 g/kg, amoxicillin (AMOX) in all solid waste samples the detection concentration is generally low, the average detection concentration of less than 0.1 g/kg. Compared with the solid waste landfill in the dawn of antibiotics detection concentration of antibiotics TCs, QNs, and MLs three kinds of antibiotics in solid waste Laogang Landfill in detected concentrations were generally lower (P0.05), SAs and BLs in solid waste landfill in two detected concentration of no significant change. In the landfill surface Laogang landfill (0.5-1.5m) of solid waste samples, showing a variation in the depth of the antibiotic concentration, except BLs the other four kinds of antibiotics (TCs, QNs, SAs, MLs) in 1.5 m depth of antibiotic detection concentration was higher than that in the depth of 0.5 m at the concentration of detection (P0.05), and the surface of solid waste landfill landfill is no dawn characteristics of the concentration distribution. This may be due to the mature stage of solid waste in the old port landfill and the downward migration and diffusion of antibiotics in rainwater and leachate. The study selected 7 antibiotic resistance genes (tetQ, tetW, mefA, ermB, sul1, sul2 and mexF) and integron INT1. Test results showed that in the landfill leachate, were detected in 7 ARGs concentration was 2.91 * 10~2 to 4.88 * 10~6 copies/ngDNA, INT1 integron detection concentration was 4.55 * 10~4 to 8.31 * 10~7 copies/ngDNA; in the landfill of solid waste, tetQ, tetM, mefA three ARGs concentration is lower than the standard curve range of quantitative detection the detection rate of ermB, sul1, sul2, and mexF four concentration of 1.85 ARGs * 102 ~ 5.07 * 106 copies/ngDNA integron INT1 detection concentration is 6.90 * 105 ~ 1.86 * 108 copies/ngDNA. Analysis of antibiotic resistance genes and the correlation between the results show that in the landfill leachate, showed a significant correlation between tetracyclines and resistance genes tetQ, ETM-H_2O, MLs and mefA have significant correlation, sulfamethoxazole (SMX), SAs and sul1 and sul2 showed a significant negative correlation, and multiple resistance genes and mexF there was no correlation between the detection of antibiotics; in Laogang surface of solid waste, only RTM and ermB have significant positive correlation, shows a significant negative correlation with multidrug resistance gene mexF; on the surface of solid waste landfill in the dawn of only sul2, and sulfadiazine (SD), sulfamethazine (SMZ) and SAs showed a significant negative correlation. This may be due to the physical and chemical properties of the environmental medium of municipal solid waste landfill (temperature, light, pH, etc.).
【學(xué)位授予單位】：華東師范大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：X799.3

【參考文獻(xiàn)】

相關(guān)期刊論文 前10條

1 朱陣;李冰;周緒正;魏小娟;程富勝;張繼瑜;;環(huán)境中細(xì)菌抗藥性的研究進(jìn)展[J];中國(guó)畜牧獸醫(yī);2016年12期

2 張?zhí)m河;王佳佳;哈雪姣;邱孟超;高敏;仇天雷;王旭明;;北京地區(qū)菜田土壤抗生素抗性基因的分布特征[J];環(huán)境科學(xué);2016年11期

3 張佳奇;徐艷;羅義;毛大慶;;重金屬協(xié)同選擇環(huán)境細(xì)菌抗生素抗性及其機(jī)制研究進(jìn)展[J];農(nóng)業(yè)環(huán)境科學(xué)學(xué)報(bào);2016年03期

4 張瀅楹;耿金菊;任洪強(qiáng);許柯;丁麗麗;;環(huán)境濃度抗生素選擇性壓力改變活性污泥微生物群落結(jié)構(gòu)[J];生態(tài)毒理學(xué)報(bào);2015年05期

5 Shiliang WANG;Hui WANG;;Adsorption behavior of antibiotic in soil environment:a critical review[J];Frontiers of Environmental Science & Engineering;2015年04期

6 李蕾;徐晶;趙由才;宋立巖;;垃圾填埋場(chǎng)抗生素抗性基因初探[J];環(huán)境科學(xué);2015年05期

7 沈怡雯;黃智婷;謝冰;;抗生素及其抗性基因在環(huán)境中的污染、降解和去除研究進(jìn)展[J];應(yīng)用與環(huán)境生物學(xué)報(bào);2015年02期

8 張立光;陸琳;宋勤琴;俞學(xué)煒;;蘇州市居民家庭過期藥品處置現(xiàn)狀調(diào)查[J];考試周刊;2015年07期

9 柯潤(rùn)輝;蔣愉林;黃清輝;陳玲;;上海某城市污水處理廠污水中藥物類個(gè)人護(hù)理用品(PPCPs)的調(diào)查研究[J];生態(tài)毒理學(xué)報(bào);2014年06期

10 楊曉洪;王娜;葉波平;;畜禽養(yǎng)殖中的抗生素殘留以及耐藥菌和抗性基因研究進(jìn)展[J];藥物生物技術(shù);2014年06期

相關(guān)碩士學(xué)位論文 前6條

1 徐莉柯;城市自來水處理系統(tǒng)中抗生素抗性基因的行為特征[D];浙江大學(xué);2015年

2 黃智婷;抗生素殘留及抗性基因在生活垃圾轉(zhuǎn)運(yùn)填埋過程中的遷移轉(zhuǎn)化和去除研究[D];華東師范大學(xué);2014年

3 葛偉麗;長(zhǎng)期施用雞糞農(nóng)田土壤中典型抗生素耐藥細(xì)菌及其抗性基因污染分析[D];山東農(nóng)業(yè)大學(xué);2014年

4 沈群輝;養(yǎng)殖場(chǎng)及周邊農(nóng)田土壤抗生素抗性基因和重金屬污染初步研究[D];東華大學(xué);2013年

5 劉娟;垃圾填埋場(chǎng)穩(wěn)定化進(jìn)程核心表征指標(biāo)研究[D];清華大學(xué);2011年

6 張小霞;海洋養(yǎng)殖水體抗藥性細(xì)菌種類及其抗藥性基因攜帶情況的研究[D];中國(guó)海洋大學(xué);2008年

，

本文編號(hào)：1340395