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博碩士論文 etd-0808115-163004 詳細資訊
Title page for etd-0808115-163004
論文名稱
Title
藥物與個人保健用品暨禁藥在高屏地區之環境流布
Occurrence of pharmaceuticals and personal care products (PPCPs) and illicit drugs in Gaoping area of Taiwan
系所名稱
Department
畢業學年期
Year, semester
語文別
Language
學位類別
Degree
頁數
Number of pages
104
研究生
Author
指導教授
Advisor
召集委員
Convenor
口試委員
Advisory Committee
口試日期
Date of Exam
2015-07-30
繳交日期
Date of Submission
2015-09-09
關鍵字
Keywords
分配係數、風險評估、禁藥、藥物與個人保健用品、新興污染物
emerging contaminants, PPCPs, illicit drugs, distribution coefficients, risk quotients
統計
Statistics
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The thesis/dissertation has been browsed 5687 times, has been downloaded 31 times.
中文摘要
本研究分析高雄屏東恆春半島三個河川流域(高屏溪、林邊溪、網紗溪)水體(溶解相與懸浮顆粒)及沉積物中所含藥物與個人保健用品暨禁藥濃度,分析方法使用固相萃取法(SPE)搭載高效能液相層析串聯質譜儀(HPLC-MS/MS)來檢測21種藥物與個人保健用品(PPCPs)以及9種禁藥的濃度。採樣時間為2011年6月與8月、2012年11月與2013年1月,探討在空間與季節分布情形可能影響的因素,及其對水環境生物影響的風險評估。
目標藥物在本研究採樣點溶解相濃度最高為caffeine(716 ng/L),偵測頻率最高為ketoprofen(100%);懸浮顆粒濃度最高為galaxolide(218 ng/g),偵測頻率100 %的有acetaminophen、ketoprofen、ampicillin、galaxolide;沉積物濃度最高則是tonalide(33.3 ng/g),偵測頻率100 %的則有acetaminophen、ibuprofen、ketoprofen、ampicillin及tonalide。
六大類藥物與個人保健用品暨禁藥中溶解相以抗生素、其他藥物及咖啡因占較高比例,懸浮顆粒與沉積物則各以個人保健用品與消炎止痛藥為主。本研究的分配係數Kd值從最低是benzophenone-4的1.84 mL/g至tonalide的6595 mL/g,Kd,ss大多略高於Kd,sed,而本研究log Koc,ss與log Koc,sed較其他研究結果來的低。
主成分分析可以發現溶解相與沉積物在林邊溪與網紗溪可能較受人為活動影響,在夏天這些區域遊客較多,因此在濕季藥物濃度較高。相關性分析方面懸浮顆粒tonalide和galaxolide與TOC為正相關。沉積物總PPCPs濃度與粒徑中值呈顯著負相關。
計算出溶解相的風險商數(Risk quotients, RQ),在本研究採樣點RQ值範圍從10-6至9.12,其中diclofenac、codeine、sulfamethoxazole、ampicillin、erythromycin-H2O的RQ值皆至少高於0.01呈現低度風險,而其中sulfamethoxazole在濕季採樣點里嶺,乾季的里嶺、高屏、雙園、羌園與林邊的RQ值大於1,林邊更高達9.12,erythromycin-H2O則是在羌園以及乾季的里嶺與高屏呈現高度風險,乾季羌園RQ值更高達6.2,這兩種藥物在這些採樣點對環境造成危害的可能呈現高度風險,須持續監測注意其對環境生物的影響。
Abstract
The occurrence and fate of pharmaceuticals and personal care products (PPCPs) and illicit drugs in surface water (dissolved phase and suspended particles) and sediments were investigated in Gaoping River, Linbian River, and Wangsha Steam from Gao-ping area of Taiwan. Samples were collected in June 2011, August 2011, November 2012, and January 2013. Samples were analyzed by solid phase extraction (SPE) and high performance liquid-chromatography coupled to tandem mass spectrometry (HPLC-MS/MS) to determine 21 PPCPs and 9 illicit drugs.
The highest concentration of PPCPs and illicit drugs in dissolved phase was caffeine (716 ng/L), and the most frequently detected compound was ketoprofen (100 %). The highest concentration of PPCPs and illicit drugs in suspended particle samples was galaxolide (218 ng/g), and four compounds (acetaminophen, ketoprofen, ampicillin, and galaxolide) were detected in all suspended particle samples. For sediments samples, the highest concentration was tonalide (33.3 ng/g), and five compounds (acetaminophen, ibuprofen, ketoprofen, ampicillin, and tonalide) were detected in all sediment samples.
Among six categories of PPCPs, antibiotics, other pharmaceuticals, and caffeine were the predominant categories in dissolved phase, while personal care products and analgesics were the predominant categories both in suspended particle and sediment. The distributions coefficients value (Kd) varied from 1.84 mL/g for benzophenone-4 to 6595 mL/g for tonalide, and the Kd,ss value were generally higher than Kd,sed. In general, log Koc values in this study were lower than those reported in the literatures.
Results from principal component analysis (PCA) indicated that the concentrations of PPCPs and illicit drugs in dissolved phase and sediment in Linbian River and Wangsha Stream might be affected by visitor population in August, and therefore, higher concentrations could be found in wet season. Correlations analysis showed a significant positive correlation between concentrations of tonalide and galaxolide in suspended particle and TOC. Total PPCPs concentrations in sediments showed a significant negative correlation with median particle size.
The results of RQ in this study ranged from 10-6 to 9.12 and showed that five compounds (diclofenac, codeine, sulfamethoxazole, ampicillin, and erythromycin-H2O) might pose at least a low risk (RQ>0.01) to aquatic organisms in this study. Sulfamethoxazole and erythromycin-H2O pose a higher risk at GP1, GP2, GP3, L1, and L2, indicating that adverse effects may occur in these sites. Additional studies of on-site toxicological data are necessary to clarify potential adverse effects in this study area.
目次 Table of Contents
謝 誌.........................................................................i
摘 要........................................................................ii
Abstract.....................................................................iv
目錄...........................................................................vi
圖目錄........................................................................ix
表目錄.........................................................................x
縮寫與代號表.............................................................xii
第一章 前言............................................................1
1.1 研究動機................................................................1
1.2 研究目的................................................................1
第二章 文獻回顧.....................................................3
2.1 藥物與個人保健用品...............................................3
2.1.1藥物與個人保健用品之基本性質.............................3
2.2 藥物與個人保健用品於環境中之來源與流布...............4
2.2.1溶解相.................................................................4
2.2.2懸浮顆粒與沉積物.................................................6
第三章 實驗方法及步驟...........................................9
3.1材料與儀器.............................................................9
3.1.1材料....................................................................9
3.1.2儀器...................................................................13
3.2 採樣與保存...........................................................13
3.2.1採樣地點............................................................13
3.2.2採樣方法............................................................13
3.3分析方法...............................................................16
3.3.1溶解相...............................................................16
3.3.2懸浮顆粒及沉積物...............................................17
3.3.3 液相層析串聯式質譜儀.......................................17
3.3.4 粒徑分析...........................................................20
3.3.5 總有機碳分析....................................................20
3.4品保及品管(QA/QC)...............................................20
3.4.1方法回收率........................................................20
3.4.2方法偵測極限.....................................................20
3.4.3實驗空白分析.....................................................21
3.5 主成分分析..........................................................21
第四章 結果與討論...............................................22
4.1空間分布..............................................................22
4.1.1溶解相藥物與個人保健用品暨禁藥濃度空間分布....22
4.1.2懸浮顆粒藥物與個人保健用品暨禁藥濃度空間分布.31
4.1.3沉積物藥物與個人保健用品暨禁藥濃度空間分布....37
4.2 季節分布.............................................................43
4.3文獻比較..............................................................51
4.3.1溶解相藥物與個人保健用品濃度文獻比較..............51
4.3.2懸浮顆粒藥物與個人保健用品濃度文獻比較...........55
4.3.3沉積物藥物與個人保健用品濃度文獻比較..............57
4.4 藥物與個人保健用品暨禁藥在各相間分布情形.........59
4.4.1各相間濃度與所占比例........................................59
4.4.2 分配係數Kd與LogKoc........................................68
4.5主成分分析與相關性分析.......................................71
4.5.1溶解相主成分分析..............................................71
4.5.2懸浮顆粒主成分分析...........................................73
4.5.3沉積物主成分分析..............................................75
4.5.4 水體中溶解相、懸浮顆粒及沉積物相關性分析......77
4.6風險評估..............................................................81
第五章 結論與建議...............................................83
5.1結論....................................................................83
5.2建議....................................................................84
參考文獻..................................................................85
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凃博文 (2012) 藥物及個人保健用品暨禁藥在台灣恆春半島西部及墾丁觀光地區之環境流布, 國立中山大學海洋環境及工程學系碩士論文.
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