【摘要】：隨著藥物及個人護(hù)理品(Pharmaceutical and personal care products,PPCPs)污染在全球環(huán)境中不斷加劇,抗生素作為其中一種分布較廣的污染物,因其對人類和生態(tài)系統(tǒng)健康構(gòu)成的嚴(yán)重的潛在威脅已廣受環(huán)境科學(xué)、毒理學(xué)及流行病學(xué)的關(guān)注。我國經(jīng)濟(jì)快速發(fā)展和人口劇增,每年消耗大量抗生素,已成為世界上最大的抗生素生產(chǎn)和使用國,水環(huán)境中的抗生素污染十分嚴(yán)峻。洞庭湖作為重要的水產(chǎn)和畜禽養(yǎng)殖區(qū)域,必然會受到一定程度的抗生素污染,但是目前對于洞庭湖抗生素的污染狀況、來源及風(fēng)險等級等鮮有報道。因此,本研究選取洞庭湖國控省控等代表性點位和12種典型抗生素,初步系統(tǒng)地研究了洞庭湖水體、沉積物及魚體中12種抗生素的賦存特征、來源及風(fēng)險等級水平,主要結(jié)果如下:(1)對現(xiàn)有的水體、沉積物和魚體樣品中的4類12種(磺胺類、磺胺增效劑、喹諾酮類和四環(huán)素類)抗生素的提取方法進(jìn)行了優(yōu)化,并進(jìn)行了方法的準(zhǔn)確度的檢驗,方法滿足水體、沉積物和魚體中目標(biāo)抗生素殘留的檢測需求;(2)洞庭湖水體中豐水期和枯水期的抗生素檢出濃度分別為ND~61.28ng·L-1和ND~8.73ng·L-1,各采樣點的抗生素總濃度分別為6.35~135.40ng·L-1和1.06~17.42 ng·L-1,季節(jié)差異顯著,磺胺類為主要污染物,以南渡、樟樹港、扁山、東洞庭湖的抗生素污染程度較高。在空間上,表現(xiàn)為東洞庭湖南洞庭湖西洞庭湖,與水產(chǎn)養(yǎng)殖、畜禽養(yǎng)殖及人口分布等密切相關(guān)。水體中抗生素的賦存還受到水體因子葉綠素a(Chla)、高錳酸鹽指數(shù)(CODMn)、TN等的影響。豐水期沉積物中抗生素的檢出濃度ND~5.56 ng·g-1,以磺胺嘧啶、恩諾沙星、金霉素、四環(huán)素為主要污染物,空間污染特征與水體基本一致。沉積物中抗生素的賦存與粒徑(ps)、沉積物容重等相關(guān)。魚體中抗生素的檢出濃度ND~1.06ng·g-1,磺胺嘧啶和恩諾沙星的檢出率較高,鯰魚、鯉魚和蝦等底層生物體內(nèi)抗生素的含量較高。(3)采用風(fēng)險熵(RQ)對洞庭湖抗生素的風(fēng)險等級進(jìn)行了評價。豐水期和枯水期水體中的主要環(huán)境風(fēng)險因子為環(huán)丙沙星、磺胺甲惡唑、恩諾沙星和沙拉沙星,對洞庭湖生態(tài)環(huán)境具有潛在的風(fēng)險;枯水期和豐水期抗生素的健康風(fēng)險值處于5.09×10-8~6.94×10-5·a-1和1.70×10-8~1.28×10-5·a-1之間,喹諾酮類為主要的健康風(fēng)險因子,風(fēng)險等級為10-6~10-5數(shù)量級,且通過飲用水?dāng)z入抗生素對成年人的健康風(fēng)險高于兒童,南渡、樟樹港等地的累積風(fēng)險較高。沉積物中10種抗生素的RQ處于2.07×10-4-29.87之間,環(huán)丙沙星、沙拉沙星為主要的風(fēng)險因子,東洞庭湖、扁山、馬坡湖、坡頭、小河嘴、樟樹港等地的累積風(fēng)險較高。洞庭湖魚體中抗生素的含量遠(yuǎn)低于最大殘留限值(MARL),城市和農(nóng)村地區(qū)通過魚蝦攝入抗生素的風(fēng)險RDQ分別處于5.85×10-7~5.17×10-4和1.23×10-6~1.09×10-3之間,恩諾沙星和沙拉沙星為主要的健康風(fēng)險因子,攝食鯰魚和蝦的健康風(fēng)險較大。(4)通過對洞庭湖周邊部分污染源的調(diào)查,初步確定了洞庭湖12種抗生素的來源。結(jié)果表明:磺胺嘧啶(SDZ)、磺胺甲惡唑(SMX)、磺胺二甲嘧啶(SMZ)、甲氧芐氨嘧啶(TMP)、沙拉沙星(SFLO)和金霉素(CTC)主要來自水產(chǎn)養(yǎng)殖和畜禽養(yǎng)殖源;環(huán)丙沙星(CIP)、土霉素(OTC)和氧氟沙星(OFL)主要來自污水處理廠;四環(huán)素主要來自于畜禽養(yǎng)殖;恩諾沙星和諾氟沙星主要來自于水產(chǎn)養(yǎng)殖。
[Abstract]:As drug and personal care products (PPCPs) pollution in the global environment continues to intensify, antibiotics as one of the widespread pollutants, because of its serious potential threat to human and ecosystem health has been widely concerned by environmental science, toxicology and epidemiology. With the rapid economic development and rapid population growth, a large number of antibiotics are consumed every year, which has become the largest antibiotic producing and using country in the world. The antibiotic pollution in the aquatic environment is very serious. The distribution, source and risk level of 12 antibiotics in Dongting Lake water, sediments and fishes were studied systematically. The main results are as follows: (1) For existing water, sediments and fishes, 12 kinds of antibiotics were selected as representative sites and 12 kinds of typical antibiotics. The extraction method of 4 kinds and 12 kinds of antibiotics (sulfonamides, sulfonamide synergists, quinolones and tetracyclines) from fish and water samples was optimized, and the accuracy of the method was tested. The method met the detection requirements of target antibiotic residues in water, sediments and fish. (2) Antibiotics in Dongting Lake during flood season and dry season. The detected concentrations were ND~61.28ng.L-1 and ND~8.73ng.L-1, respectively. The total concentrations of antibiotics in each sampling site were 6.35~135.40ng.L-1 and 1.06~17.42 ng.L-1, respectively. The seasonal difference was significant. Sulfonamides were the main pollutants. The antibiotics in Nandu, Zhangshugang, Bianshan and Dongdongting lakes were highly contaminated. Xidongting Lake is closely related to aquaculture, livestock and poultry breeding and population distribution. The occurrence of antibiotics in the water body is also affected by the water body factors such as chlorophyll a (Chla), permanganate index (CODMn), TN and so on. The occurrence of antibiotics in sediments was related to particle size (ps) and bulk density of sediments. The detection concentration of antibiotics in fish was ND~1.06ng g-1, the detection rate of sulfadiazine and enrofloxacin was higher, and the content of antibiotics in catfish, carp and shrimp was higher. (3) Risk Entropy (RQ) The risk grade of antibiotics in Dongting Lake was evaluated. The main environmental risk factors in the high and low water periods were ciprofloxacin, sulfamethoxazole, enrofloxacin and sarafloxacin, which had potential risks to the ecological environment of Dongting Lake. Quinolones were the main health risk factors, and the risk level was 10-6-10-5. The cumulative risk of antibiotics ingested through drinking water was higher in adults than in children, Nandu, Zhangshugang and other places. Salafloxacin was the main risk factor, and the cumulative risk was higher in Dongting Lake, Bianshan, Mapo Lake, Potou, Xiaohezui and Zhangshu Harbor. The antibiotic content in Dongting Lake fish was much lower than the maximum residue limit (MARL), and the risk RDQ of antibiotic intake by fish and shrimp in urban and rural areas was 5.85 *10-7~5.17 *10-4 and 1.23 *10-6~1, respectively. Enrofloxacin and sarafloxacin were the main health risk factors, and catfish and shrimp were the main health risk factors. (4) The sources of 12 antibiotics in Dongting Lake were preliminarily determined by investigating some pollution sources around Dongting Lake. The results showed that sulfadiazine (SDZ), sulfamethoxazole (SMX), sulfamethoxazole (SMZ), trimethoprim (TMZ). Aminopyrimidine (TMP), Sarafloxacin (SFLO) and aureomycin (CTC) are mainly from aquaculture and poultry breeding sources; ciprofloxacin (CIP), oxytetracycline (OTC) and ofloxacin (OFL) are mainly from sewage treatment plants; tetracycline is mainly from livestock and poultry breeding; enrofloxacin and norfloxacin are mainly from aquaculture.
【學(xué)位授予單位】：山東師范大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：X52;X824

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