利用無溶劑萃取技術快速測定環境固態樣品中之多環類麝香化合物的研究

以作者查詢圖書館館藏

、以作者查詢臺灣博碩士

、以作者查詢全國書目

、勘誤回報

、線上人數：46

、訪客IP：3.144.102.156

姓名

吳欣芳(Shin-Fang Wu) 查詢紙本館藏

畢業系所

化學學系

論文名稱

利用無溶劑萃取技術快速測定環境固態樣品中之多環類麝香化合物的研究
(Fast Determination of Synthetic Polycyclic Musks in Solid Samples by Solvent Free Techniques)

相關論文

★ 以質譜技術探討非共價鍵結蛋白質聚合物之結構	★ 以液相層析質譜儀檢測水樣與生物檢體中全氟界面活性劑之濃度
★ 利用液相層析串聯質譜技術檢測水環境中藥物殘留物之方法開發與應用	★ 以MIL-101(Cr)作為吸附劑結合MALDI-TOF-MS快速檢測環境水樣中二苯甲酮類化合物的殘留
★ 直鏈式烷基苯基二甲基銨鹽類陽離子型界面活性劑在水環境中微量檢測方法的研究	★ 芳香族磺酸鹽類有機污染物在水環境中的分析與研究
★ 以固相萃取及氣相層析質譜儀對水環境中壬基苯酚類持久性有機污染物之分析與研究	★ 以固相萃取法及氣相層析質譜儀對水環境中動情激素類有機污染物之分析與研究
★ 利用熱裂解直接高溫衍生化法快速分析直鏈式烷基三甲基銨鹽之方法建立與探討	★ 利用感應偶合電漿質譜儀檢測半導體製程用化學品中微量金屬不純物之分析研究
★ 應用毛細管電泳間接偵測方法分離四級銨鹽界面活性劑	★ 利用毛細管電泳結合線上濃縮方法分離奈磺酸鹽之機制探討
★ 快速分析水環境中醫療藥品殘留物之研究與探討	★ 以毛細管電泳法與電灑游離質譜法探討內包錯合物之研究
★ 以氣相及液相層析質譜儀分析具荷爾蒙效應物質之方法開發	★ 以離子配對高效液相層析儀檢測螢光增白劑在不同基質中之研究

檔案

[Endnote RIS 格式]

[Bibtex 格式]

[相關文章]

[文章引用]

[完整記錄]

[館藏目錄]

[檢視]

[下載]

本電子論文使用權限為同意立即開放。
已達開放權限電子全文僅授權使用者為學術研究之目的，進行個人非營利性質之檢索、閱讀、列印。
請遵守中華民國著作權法之相關規定，切勿任意重製、散佈、改作、轉貼、播送，以免觸法。

摘要(中)

從古代開始，香氛就經常被用來增加對於個人的吸引力，而麝香因為在香精工業中被大量使用而佔有一席之地。多環類合成麝香作為天然麝香的平價替代品，在生產製造過程以及一般大眾使用後會隨著污水處理廠處理過後的污水及污泥排放到環境當中，而主要的污染源頭即為這些廢污水以及污泥。
本篇研究中，利用一步完成的微波輔助頂空固相微萃取裝置搭配氣相層析質譜儀分析廢污泥、沉積物以及牡蠣樣品，方法不僅快速且不須使用有機溶劑。將除水後的固態樣品與20毫升的去離子水混合，以PDMS-DVB的塗附纖維置於樣品頂空後，使用80瓦微波，萃取5分鐘。此方法的偵測極限為0.04至0.1 ng/g，而定量極限為0.1至0.3 ng/g。
對於這些環境樣品的初步檢測結果顯示，HHCB以及AHTN為最普遍被
檢測到的兩種多環類麝香化合物，利用標準添加法進行定量分析，待測物的總濃度介於0.3至10.9 ng/g，而再現性的相對標準偏差範圍為4 %至10 %。
本實驗所開發的微波輔助頂空固相微萃取法，搭配氣相層析質譜儀的選擇離子掃描偵測模式，為一種具有可靠性且靈敏度高的檢測方法，提供了一個方便的檢測技術以檢測環境固態樣品中微量的多環類麝香化合物。

摘要(英)

Fragrances have been used increase attractiveness of persons since ancienttimes. Musk is one of the most important and often used fragrances in perfumery. Synthetic polycyclic musks are inexpensive substitutes for natural musks. Synthetic polycyclic musk compounds enter environment principally through effluents of wastewater treatment plants and waste sludge, and the major source of environmental pollution of synthetic musks is from sewage.
In this study, one-step in situ microwave-assisted headspace solid-phase microextraction (MA-HS-SPME) followed by gas chromatography-mass spectrometry (GC-MS) analysis is presented as a fast and solvent-free technique
to determine synthetic polycyclic musks in sewage sludge, sediment and oyster samples. The dewatered solid sample mixed with 20-mL deionized water was efficiently extracted by a polydimethylsiloxane-divinylbenzene (PDMS-DVB)
fiber placed in the headspace when the extraction slurry was microwave irradiated at 80 W for 5 min. The limits of detection (LODs) ranged from 0.04 to 0.1 ng/g, and the limits of quantification (LOQs) ranged from 0.1 to 0.3 ng/g
(fresh weight).
A preliminary analysis of those samples revealed that HHCB and AHTN were the two most commonly detected synthetic polycyclic musks; using a standard addition method, their total concentrations were determined to rangefrom 0.3 to 10.9 ng/g (fresh weight) with relative standard deviation (RSD)ranging from 4% to 10%.
The analytical procedure developed demonstrated that the MA-HS-SPME and GC-MS-SIM methods are reliable, sensitive and offer a convenient analytical technique for trace determination of polycyclic musks in various solid
samples in environment.

關鍵字(中)

★ 氣相層析質譜儀
★ 多環類麝香
★ 固相微萃取法

關鍵字(英)

★ Polycyclic Musks
★ GC-MS
★ SPME

論文目次

第一章　前言 1
1-1　研究緣起 1
1-2　研究目標 5
第二章　文獻回顧 6
2-1　新興污染物 6
2-1-1　新興污染物的來源及環境流佈 6
2-1-2　多環類麝香化合物簡介 10
2-1-3　多環類麝香化合物的毒性與物化性質 12
2-1-4　多環類麝香化合物的污染現況 17
2-1-5　相關研究文獻 19
2-2　微波輔助萃取法 22
2-2-1　微波簡介 22
2-2-2　加熱原理 24
2-2-3　微波裝置 26
2-2-4　微波的應用 27
2-3　固相微萃取法 30
2-4　氣相層析質譜儀 35
2-4-1　四極矩質譜儀 38
2-4-2　選擇離子偵測法 39
2-5　標準添加法 40
第三章　實驗步驟與樣品分析 43
3-1　實驗藥品與設備 43
3-1-1　實驗藥品 43
3-1-2　儀器設備 44
3-2　實驗步驟 46
3-2-1　標準品的配製 46
3-2-2　氣相層析質譜儀的參數設定 46
3-2-3　MA-HS-SPME裝置示意圖 48
3-2-4　微波輔助頂空固相微萃取步驟 49
3-3　樣品採集 50
3-2-1　底泥採集 50
3-2-2　牡蠣樣品收集 50
3-4　真實樣品檢測定量步驟 51
第四章　結果與討論 52
4-1　氣相層析質譜儀對多環類麝香化合物之分析 52
4-1-1　多環類麝香化合物標準品的測定 52
4-1-2　多環類麝香化合物標準品的儀器偵測極限與線性範圍 57
4-2　微波輔助萃取條件最佳化 58
4-2-1　微波瓦數對於萃取量的影響 58
4-2-2　萃取時間對於萃取量的影響 59
4-3　模擬樣品的最佳化 61
4-3-1　萃取溶劑體積對於萃取量的影響 61
4-3-2　NaCl添加量 62
4-3-3　pH值對於萃取量的影響 64
4-4　微波輔助頂空固相微萃取法的最佳化結果 66
4-3-3　微波輔助頂空固相微萃取法之最佳化條件 66
4-4-3　微波輔助頂空固相微萃取法之檢量線 67
4-5　微波輔助萃取法與傳統萃取方法的比較 69
4-6　環境樣品中多環類麝香的定量分析 71
4-6-1　底泥樣品中多環類麝香化合物的測定 71
4-6-2　牡蠣樣品中多環類麝香化合物的測定 77
第五章　結論與建議 79
5-1　結論 79
5-2　建議 80
第六章　參考文獻 81

參考文獻

? 中華民國財政部關稅總局，進出口數量統計(http://web.customs.gov.tw/statistic/statistic/statisticlist.asp)
? 環保署環境檢驗所：底泥採集方法 NIEA S102.61B，民國92年。
? 陳崇宇、李茂榮：微波萃取技術之應用，科儀新知，民國92年。
? 王妤甄：以微波輔助頂空固相微萃取法萃取水樣中的多環麝香化合物，民國98年。
? 吳信宏：以為剝輔助萃取搭配液相層析質譜儀檢測固態樣品中六溴環十二烷之方法開發，民國97年。
? Artola-Garicano, E.; Borkent, I.; Hermens, J.M.; Vaes,W.J., Removal of Two Polycyclic Musks in Sewage Treatment Plants: Freely Dissolved and Total Concentrations, Environ. Sci. Technol., 2003, 37, 3111-3116.
? Balk, F.; Ford, R.A., Environmental risk assessment for the polycyclic musks AHTN and HHCB in the EU: Ⅰ. Fate and exposure assessment, Toxicol. Lett., 1999, 111, 57-79.
? Bitsch, N.; Dudas, C.; Körner, W.; Failing, K.; Biselli, S.; Rimkus, G.G.; Brunn1, H., Estrogenic Activity of Musk Fragrances Detected by the E-Screen Assay Using Human MCF-7 Cells, Arch. Environ. Contam. Toxicol., 2002, 43, 257–264.
? Chou, Y-J; Dietrich, D.R., Toxicity of nitromusks in early lifestage of south african clawed frog (Xenopus laevis) and zebrafish (Danio rerio), Toxicol. Lett., 1999, 11, 17-25.
? Difrancesco,A.M.; Chiu,P.C.; Standley, L.J.; Allen,H.E.; Salvito,D.T., Dissipation of Fragrance Materials in Sludge-Amended Soils, Environ. Sci.Technol., 2004, 38, 194.
? Fromme, H.; Otto, T.;Pilz, K.,Polycyclic musk fragrance in different environmental compartments in Berlin(Germany).Water Res., 2001,
35(1),121-128.
? Gatermann, R.; Hellou, J.; Huhnerfuss, H.; Polycyclic and nitro musks in the environment：A comparison between Canada and European aquitic biota.,Chemosphere, 1999, 38(14), 3441-3441.
? Gatermann, R.; Biselli, S.; Hűhnerfuss, H.; Rimkus, G.G.; Hecker, M.; Karbe, L., Sythetic musks in the environmennt. Part 1: Species-dependent bioaccumulation of polycyclic and nitro musk fragrances in freshwater fish and mussels, Arch. Environ. Con. Tox., 2002, 42, 437-446.
? Giddings, J.M.; Salvito, D.; Putt, A.E., Acute toxicity of 4-amino musk xylene to daphnia magna in laboratory water and natural water, Water Res., 2000, 34, 3686-3689.
? Glassmeyer, S.T., The cycle of emerging contaminants, Water Resour. IMPACT, 2007, 9, 5-7.
? Hájlová, K.; Pulkrabová, J.; Hajšlová, J.; Randák, T.; Žlábek, V., Chub (Leuciscus cephalus) as a Bioindicator of Contamination of the Vltava River by Synthetic Musk Fragrances, Arch. Environ. Contam. Toxicol., 2007, 53, 390–396.
? Harris, D.C., Quantitative chemical analysis, 6th ed., W.H. Freeman and Company, 2002.
? Heberer, T., Occurrence, Fate, and Assessment of Polycyclic Musk Residues in the Aquatic Environment of Urban Areas – A Review, Acta hydrochim. hydrobiol., 2002, 30, 5–6, 227–243.
? Heberer, T.; Gramer, S.; Stan, H-J., Occurrence and distribution of organic contaminants in the aquatic system in Berlin, Germany. Part 3. Determination of synthetic musks in Berlin surface water applying solid-phase microextraction (SPME) and gas chromatography-mass spectrometry (GC-MS), Acta Hydroch. Hydrob., 1999, 27, 150-156.
? Holtz, S., There is no “Away.” Pharmaceuticals, personal care products, and endocrine-disrupting substances: Emerging contaminants detected in water, Canadian institude for environmental law and policy, 2006.
? Kallenborn, R.; Gatermann, R., Synthetic Musks in Ambient and Indoor Air, The Handbook of Environmental Chemistry, 2004, 3, 85–104.
? Kannan, K.; Reiner, J.L.; Yun,S.H.; Perrotta, E.E.; Tao, L.; Johnson-Restrepo, B.; Rodan, B.D., Polycyclic musk compounds in higher trophic level aquatic organisms and humans from the United States., Chemosphere, 2005, 61, 693.
? Kupper, T.; Berset, J.D.; Etter-Holzer, R.; Furrer, R.; Tarradellas, J.,
Concentrations and specific loads of polycyclic musks in sewage sludge originating from a monitoring network in Switzerland., Chemosphere, 2004, 54, 1111-1120.
? Lignell, S; Darnerud, P.O.; Aune, M.; Cnattingius, S.; Hajšlová, J.; Setkova, L.; Glynn, A., Temporal Trends of Synthetic Musk Compounds in Mother′s Milk and Associations with Personal Use of Perfumed Products., Environ. Sci. Technol., 2008, 42, 6743-6748.
? Luckenbach, T. ; Epel, D., Nitromusk and Polycyclic Musk Compounds as Long-Term Inhibitors of Cellular Xenobiotic Defense Systems Mediated by Multidrug Transporters, Environ. Health Perspect., 2005, 113, 17–24.
? McCarty, L.S.; Mackay, D.; Smith, A.D.; Ozburn, G.W.; Dixon, D.G., Residue-based interpretation of toxicity and bioconcentration QSARs from aquatic bioassays: Neutral narcotic organics, Environ. Toxico. Chem., 1992, 11, 917-930.
? Müller, S,; Schmid, P.; Schlatter, C., Occurrence of nitro and non2nitro
benzenoid musk compounds in human adipose tissue., Chemosphere, 1996, 33, 17-28..
? Pedersen, S.; Selck, H.; Salvito, D.; Forbes, V., Effects of the polycyclic musk HHCB on individual- and population-level endpoints in Potamopyrgus antipodarum, Ecotoxicol. Enviro. Saf., 2009, 72, 1190–1199.
? Petrović, M.; Gonzale, S.; Barceló, D., Analysis and removal of emerging contanminants in wastewater and drinking water, Trends Anal. Chem., 2003, 22, 685-696.
? Pomati, F.; Catiglioni, S.; Zuccato, E.; Fanelli, R.; Vigetti, D.; Rossetti, C.; Calamari, D., Effects of a complexmixture of therapeutic drugs at environmental levels on human embryonic cells., Environ. Sci. Technol., 2006, 40, 2442–2447.
? Rimkus, G. G.; Wolf, M., Polycyclic musk fragrances in human adipose tissue and human milk, Chemosphere, 1996, 33(10), 2033-2043.
? Rimkus, G. G., Polycyclic musk fragrances in the aquatic environment, Toxicol. Lett., 1999, 111, 37-56.
? Rubinfeld, S.A.; Luthy, R.G., Nitromusk compounds in San Francisco Bay sediments., Chemosphere, 2008, 73, 873-879.
? Rüdel, H.; Böhmer, W.; Schröter-Kermanib, C., Retrospective monitoring of synthetic musk compounds in aquatic biota from German rivers and coastal areas., J. Environ. Monit., 2006, 8, 812-823.
? Schnell, S.; Bols, N. C.; Barata, C.; Cinta Porte, C., Single and combined toxicity of pharmaceuticals and personal care products (PPCPs) on the rainbow trout liver cell line RTL-W1, Aquat. Toxicol., 2009, 93, 244–252.
? Seinen, W.; Lemmen, J. G.; Pieters, R. H. H.; Verbruggen, E.M.J.; van der Burg, B., AHTN and HHCB show weak estrogenic – but no uterotrophic activity, Toxicol. Lett., 1999, 111, 161-168.
? Silva, A. R. M.; Nogueira, J. M. F., Stir-bar-sorptive extraction and liquid desorption combined with large-volume injection gas chromatography–
mass spectrometry for ultra-trace analysis of musk compounds in environmental water matrices, Anal.Bioanal. Chem., 2010, 369, 1853-1862.
? Simonich, S.; Federle, T.W.; Eckhoff, W.S.; Rottiers, A.; Webb, S.; Sabaliunas, D.; Wolf, W., Removal of fragrance materials during U.S. and European wastewater treatment., Environ. Sci. Technol., 2002, 36, 2839-2847.
? Skoog, D.A.; Holler, F.J.; Crouch, S.R., Principles of instrumental analysis, 6th ed., Thomson Learning, 2006.
? Sommer, C., The Role of Musk and Musk Compounds in the Fragrance Industry, The Handbook of Environmental Chemistry, 2004, 3, 1-16.
? Spencer, P.S.; Bischoff-Fenton, M.C.; Moreno, O.M.; Opdyke, D.L.; Ford, R.A., Neurotoxic properties of musk ambrette, Toxicol. Appl. Pharm., 1984, 75, 571-575.
? Steven, J.L.; TEVEN J，Northcot, G.; Stern, G.A.; Tomy, G.T.; Jones, K.C., PAHs, PCBs, PCNs, organochlorine pesticides, synthetic musks, and
polychlorinated n-alkanes in U.K. sewage sludge: survey results and
implications., Environ. Sci. Technol., 2003, 37, 462-467.
? Sumner, N.R.; Guitart, C.; Fuentes, G.; Readman, J.W., Inputs and distributions of synthetic musk fragrances in an estuarine and coastal environment; a case study., 2010, Environmental Pollution, 215–222.
? Tas, J.W.; Balk, F.; Ford, R.A.; van der Plassche, E.J., Environmental risk assessment of musk ketone and musk xylene in the netherlands in accordance with the EU-TGD, Chemosphere, 1997, 35, 3686-3715.
? Ternes, A.T.,Joss,A.;Siegrist, H., Scrutinizing pharmaceuticals and personal care products in wastewater treatment, Environ. Sci. Technol., 2004, 38, 393-399.
? Yamagishi, T.; Miyazaki, T.; Horri, S., Kaneki Identification ofmusk xvlene and musk ketone in freshwater fish collected from the Tama River Tokyo.Bull Environ. Contam. Toxicol., 1981, 26, 656-662.
? Zeng, X.Y.; Sheng, G.Y.;Gui, H.Y., et al. 2007. Preliminary study on the
occurrence and distribution of polycyclic musks in a wastewater
treatment plant in Guandong, China., Chemosphere, 2007, 69,
1305-1311.
? Zhang, Z.; Pawliszyn, J., Headspace solid-phase microextraction, Anal. Chem., 1993, 65, 1843-1852

指導教授

丁望賢(Wang-Hsien Ding)

審核日期

2010-6-23

推文