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  • 學位論文

藥物與個人保健用品於污水與淨水處理程序中分佈與宿命之探討

Occurrence and Fate of Pharmaceuticals and Personal Care Products during Wastewater and Drinking Water Treatment Processes

指導教授 : 李公哲
共同指導教授 : 林郁真(Angela Yu-Chen Lin)

摘要


新興污染物為「新認定或之前未確認」、「未受法規規範」且「對人體健康及生態環境具有風險性」的化學污染物,如:藥物與個人保健用品、內分泌干擾物質、工業用化學物質及廢水排放之有機污染物。藥物與個人保健用品與人類日常生活密切相關,尤其經由飲用水作為直接進入身體的暴露途徑,其所產生的人體風險不可小覷;此外,雖然藥物與個人保健用品在環境中的濃度極低(ng/L等級),但仍會對環境產生潛在之風險。近年來許多研究指出,藥物與個人保健用品無法在傳統的淨水處理場及二級污水處理廠中有效去除。本研究目的為:1) 調查六十一種藥物與個人保健用品(包含抗生素、β-促效劑、中樞神經興奮劑、血管擴張劑、精神疾病用藥、非類固醇類消炎藥、潰瘍抑制劑及血脂抑制劑)於污水處理廠之主要處理程序及淨水處理場中進流與放流的分佈及宿命。2) 計算選定的目標化合物於污水處理廠之去除效率。3) 調查選定之目標化合物於水樣中基質干擾造成之離子抑制及離子強化效應。 本研究應用固相萃取技術(SPE)及高效能液相層析串聯質譜儀(HPLC-MS/MS)分析目標化合物。污水處理廠中sulfonamide類抗生素進流濃度範圍為7至815 ng/L,tetracyclines, β-lactam及cephalosporins類抗生素偵測到之最高進流濃度為2534,19333 及 41067 ng/L,而caffeine及非類固醇類消炎藥為污水中具最高平均濃度之化合物,分別為24467及33400 ng/L。大部分之目標化合物在污水處理二級處理程序中有較佳的去除效率,而消毒程序方面,其中一家污水處理廠應用紫外光(UV)消毒法去除sulfamethoxazole效率高達88%,其餘五家污水處理廠使用加氯消毒法其去除效率僅有20%至59%。整體而言,cephalosporins類抗生素,caffeine及非類固醇類消炎藥在調查之大部分污水處理廠中可有效去除(> 93%)。此外,藥物化合物在淨水處理場中測得之濃度極低(未測得至0.8 ng/L),除了進流曾偵測到cloxacillin濃度高達2447 ng/L,以及cefazolin與ibuprofen在放流濃度分別為318 ng/L及185 ng/L。 水樣中的基質干擾(離子化抑制/增強)會影響分析訊號,使偵測到的目標化合物放流濃度提高,包含目標物中的sulfamethoxazole, erythromycin-H2O, clarithromycin, cefazolin, ibuprofen, diclofenac, clofibic acid 和 gemfibrozil (污水處理廠)及cefazolin (淨水處理場):1)第一種情況為進流與放流水樣皆有離子化抑制現象,但進流水樣的訊號強度抑制程度較多:erythromycin-H2O, clarithromycin, ibuprofen, diclofenac, clofibic acid and gemfibrozil, 2)放流水樣離子化被增強而進流水樣則有離子化抑制現象:sulfamethoxazole, 3)進流與放流水樣皆有離子化增強現象,但放流水樣的訊號強度增強程度較多:cefazolin。本研究每一批次的基質干擾實驗,所有的目標化合物皆在具有相同背景水樣條件下進行,因此基質干擾對於目標物影響的差異可能決定於目標化合物的物理及化學特性。此外,fenoprofen (污水處理廠), chlortetracycline及erythromycin-H2O(淨水處理場)的放流濃度皆有提高的現象,而本研究證實其與水樣中的基質干擾無關,因此不易去除且殘存於水處理程序中的fenoprofen, chlortetracycline及erythromycin-H2O為值得關切的重要議題。

並列摘要


Pharmaceuticals and personal care products (PPCPs) is an important group of chemicals of emerging concerns due to their possible health effects to organism (drinking water is regarded as the most direct route entering human body) and potential risk to environment even at the low concentrations (ng/L). Recent researches indicate that PPCPs were not efficiently removed in both secondary wastewater treatment plants (WWTPs) and conventional drinking water treatment plants (DWTPs). The aims of the study were to: 1) investigate the occurrence and fate of sixty-one PPCPs simultaneously (include antibiotics, β-agonists, psychostimulants, vasodilators, psychiatric drugs, non-steroidal anti-inflammatory drugs (NSAIDs), antiulcer agent and lipid regulator) during treatment processes in WWTPs and influents and effluents in DWTPs, and 2) evaluate the removal efficiency of target PPCPs in six WWTPs, and lastly 3) examine the matrix interferences causing ion suppression and ion enhancement of target PPCPs in analyzing water samples. In this study, high performance liquid chromatography–tandem mass spectrometry (HPLC-MS/MS) was performed to analyze the target compounds after solid phase extraction. The detected influent concentrations in WWTPs ranged from 7-815 ng/L for sulfonamide antibiotics, and up to 2534, 19333 and 41067 ng/L for tetracyclines, β-lactam, and cephalosporins antibiotics. Psychostimulants (caffeine) and NSAIDs were detected at highest concentrations (up to 24467 and 33400 ng/L, respectively). The majority of target compounds were found to be eliminated to a relatively higher degree in the secondary treatment process. In disinfection process, sulfamethoxazole was 88% eliminated in one of the WWTPs which applies ultraviolet (254 nm) treatment; in other WWTPs when chlorination was applied, lower removal efficiencies (20-59%) were observed. Cephalosporins antibiotics, caffeine and NSAIDs were removed effectively (> 93%) in most of WWTPs. Most of the PPCPs were detected in DWTPs with low concentrations [not detected (ND)-88 ng/L] except for cefazolin (318 ng/L, effluents), cloxacillin (2447 ng/L, influents) and ibuprofen (185ng/L, effluents). Matrix interferences occurred for sulfamethoxazole, erythromycin-H2O, clarithromycin, ibuprofen, diclofenac, clofibic acid and gemfibrozil (WWTP) and cefazolin (DWTP) resulting in high detected effluent concentrations: 1) anlayte responses of effluent samples were suppressed to the less degree than that of influent samples, 2) anlayte responses of influent water samples were suppressed but enhanced in that of effluent water samples compared with that of D.I. water (25% MeOH), and 3) anlayte responses of effluent samples were enhanced to the more degree than that of influent samples. Each batch of matrix interference experiments in this study was on the same matrix source condition, consequently the matrix interferences caused in some of the PPCPs samples might depend on the PPCPs physic-chemical properties. Furthermore, the increasing effluent concentrations of fenoprofen (WWTPs), chlortetracycline and erythromycin-H2O (DWTPs) do not result from matrix interferences. It demonstrated that fenoprofen, chlortetracycline and erythromycin-H2O are stable and persistent during the water treatment processes which warren future attentions.

參考文獻


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被引用紀錄


吳孟純(2012)。污水處理廠去除個人防護用品及放流水質對承受水體之評估探討〔碩士論文,國立屏東科技大學〕。華藝線上圖書館。https://doi.org/10.6346%2fNPUST.2012.00270

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