研究生: |
粘弘吉 Nian, Hungchi |
---|---|
論文名稱: |
分析技術開發及應用研究: Part I.自動瞬時量測空氣與水中微量揮發性有機物之分析研究; Part II.以高壓萃取法萃取斑蟊與芭樂葉中有效成分及生物活性之研究 Development and Application of Analytical Technique: Part I. The Studies of Automatic In-situ Monitoring of Volatile Organic Compounds in the Ambient and Wastewater; Part II. The Studies of Bioactive Compounds of Mylabris and Guava Leaves Extracted by Pressurized Extraction |
指導教授: |
羅俊光
Lo, Jiunn-Guang 瞿港華 Chiu, Kong-Hwa |
口試委員: | |
學位類別: |
博士 Doctor |
系所名稱: |
原子科學院 - 生醫工程與環境科學系 Department of Biomedical Engineering and Environmental Sciences |
論文出版年: | 2009 |
畢業學年度: | 98 |
語文別: | 中文 |
論文頁數: | 226 |
中文關鍵詞: | 揮發性有機物 、瞬時量測 、高壓萃取法 、斑蟊 、芭樂 |
相關次數: | 點閱:3 下載:0 |
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本研究論文為分析技術開發及應用之研究,共分為兩部份:第一部份--自動瞬時量測空氣與水中微量揮發性有機物之分析研究。本研究空氣監測部分利用實驗室開發完成的自動化氣相層析質譜儀,建立自動採樣分析之氣相層析質譜系統,進行連續十一天之環境監測,期間納莉颱風侵襲本島,儀器仍持續正常運作。颱風滯留三天裡,量測丙酮濃度低至偵測極限以下;相對極性較低之物種而言,甲苯平均濃度值為3.0 ppbv。得知極性高之物質容易隨著雨水沖刷而流至地面,雨量之多寡將對極性物種與非極性物種之量測有著不同程度影響。
另外,本研究水體監測部份針對經污水處理廠處理後廢水中揮發性有機化合物進行監測系統建立及分析,研究中監測系統發展為完全自動進樣、自動化的分析系統,有效縮短分析時間且運用在現場即時監測,有效取得24小時連續即時的分析結果並節省現場採樣、人力分析與資源的運用。
第二部份--以高壓萃取法萃取斑蟊與芭樂葉中有效成分及生物活性之研究。在斑蝥素的萃取上, CO2搭配乙腈約萃取出9.18 mg/g斑蝥素。液態二氧化碳萃取斑蝥素的與傳統的萃取方法有較明顯的差別,雖說效果並非最佳的萃取方法,但其主要優點是可以減少有機溶劑的使用,縮短萃取時間(液態二氧化碳30min;傳統萃取需65小時)並且幾乎不需要再經由其他純化的步驟就可以得到斑蝥素。
在芭樂葉萃取方法中,以高壓甲醇萃取法有較好的總類黃酮萃取效率,而其中利用加壓萃取不但省時而且省溶劑,所以實驗的萃取方式採用高壓甲醇萃取法。在動物餵食測試推論出quercetin對於芭樂葉降血糖的能力有一定的幫助,但是並非芭樂葉降血糖主要的有效成分,應該還有其他更重要的活性成分導致在動物實驗中明顯的降血糖效果。
The thesis contained two parts. In the first part, automatic in-situ monitoring systems of volatile organic compounds (VOCs) in the ambient and wastewater were developed.The study describes continual monitoring of the volatile organic air pollutants, acetone and toluene, in HsinChu Science Park (HSP) during an inclement weather occurrence, i.e., typhoon. A total of 53 polar and nonpolar compounds were identified and analyzed. The method detection limit (MDL) was 0.4 ppbv on average. The study presents a novel system, which continuously monitors polar VOCs in industrial wastewater. The system utilizes an ultrasound coupled autosampler, headspace solid-phase microextraction (HS-SPME), and a gas chromatography/flame ionization detection GC/FID for onsite, real-time detection and quantification of VOCs. The MDL was between 3.19ppb and 7.57ppb.
In another part, the study using pressurized liquid carbon dioxide to extract cantharidin from Mylabris was investigated. The result achieves green extraction of bioactive ingredients in the insect, and the extraction efficiency of 95% (three times) was obtained at pressure of 1 MPa, temperature of 60°C, static extraction time of 30 minutes and with 4 ml of acetonitrile as modifier. In addition to the identification of the extract, i.e., cantharidin, by chromatographic approach, an in vitro assay for the effect of the extract on the cell was performed, the result reveals that the cantharidin-extracted is efficacious for primary medicinal available.
The study proposes to verify the hypoglycemic effect of the flavonoids extracted from guava leaves on type 2 diabetic mice. When comparing the total flavonoid contents from various extraction methods, pressurized-methanol extraction had the highest levels (38.4±1.5 mg g-1). The major flavonoids of guava leaves were analyzed with mass spectrometry (MS) coupled with a high-performance liquid chromatograph, diode-array detector (HPLC-DAD). To confirm the hypoglycemic effect, an animal fasting test was conducted. In summary, both primary extracts (dose of 0.5 g Kg-1) and isolated flavonoids (dose of 40 mg Kg-1) from guava leaves had hypoglycemic effects (P<0.001). However, the quercetin flavonoid in guava leaves was only one of the active compounds with hypoglycemic activity, not the most major active compound.
1. 行政院環保署環境檢驗所, 不□鋼採樣筒/氣相層析質譜儀法, NIEA A715.11B,2000. (http://www.niea.gov.tw/scripts/epa_niea/ListMethod.asp?methodtype=AIR)
2. U.S. EPA. Compendium method TO-14A, The determination of volatile organic compounds (VOCs) in ambient air using specially prepared canisters with subsequent analysis by gas chromatography; 1999.
3. U.S. EPA. Compendium method TO-15, The determination of volatile organic compounds (VOCs) in air collected in specially prepared canisters and analyzed by gas chromatography/mass spectrometry(GC/MS); 1999.
4. U.S. EPA. Compendium method TO-16, Long-path open-path Fourier transform infrared monitoring of atmospheric gases; 1996.
5. U.S. EPA. Compendium method TO-17, The determination of volatile organic compounds (VOCs) in air using active sampling onto sorbent tubes; 1997.
6. Zimmerman, P.R. Testing of Hydrocarbon Emissions from Vegetation, Leaf Litter, and Aquatic Surfaces, and Development of A Methodology for Compiling Biogenic Emission Inventories”, EPA-450/4-70-004, U.S. EPA, Washington, D.C, 1979.
7. McClenny, W. A.; Pleil, J. D.; Evans, G. F. ; Oliver, K. D.; Holdren, M. W.; Winberry, W. T. J. Air Waste Manage. Assoc. 1991, 41, 1308.
8. Gholson, A. R.; Jayanty, R. K. M.; Storm, J. F. Anal. Chem. 1990, 62, 1899.
9. Brymer, D. A.; Ogle, L.D.; Jonse, C. J.; Lewis, D.L. Environ. Sci. Technol. 1996, 30, 188.
10. 凌永健,洪長春,鄧慧卿,雷逸智,環境分析用質譜儀,科儀新知,17(5),25(1996).
11. 王碧,氣相層析質譜術在環境分析上的應用,質譜分析術專輯,國科會精密儀器發展中心,141(1992).
12. Hughes, E. E.; Davenport, A. J.; Wood P. T.; Zielinski, W. L. Environ. Sci. Technol. 1991, 25, 671.
13. Magdalena Ligor, Boguslaw Buszewski,“Determination of menthol and menthone in food and pharmaceutical products by solid-phase microextraction–gas chromatography”Journal of Chromatography A 1999, 847,161-169
14. Beatriz Cancho, Francesc Ventura, M Teresa Galceran,“Determination of aldehydes in drinking water using pentafluorobenzylhydroxylamine derivatization and solid-phase microextraction”Journal of Chromatography A 2001, 43,1-13
15. Watson Susan B., Brian Brownlee, Trevor Satchwill, Erika E. Hargesheimer,“Quantitative analysis of trace levels of geosmin and MIB in source and drinking water using headspace SPME”Water Research 2001, Vol.34,2818-2828
16. Page B. Denis, Gladys Lacroix,“Application of solid-phase microextraction to the headspace gas chromatographic analysis of semi-volatile organochlorine contaminants in aqueous matrices”Journal of Chromatography A 1997, 757, 173-182
17. Neppolian B., Haeryong Jung, Heechul Choi, Jai H. Lee, Joon-Wun Kang,“Sonolytic degradation of methyl tert-butyl ether: the role of coupled fenton process and persulphate ion”Water Research 2002, Vol.36,4699-4708
18. Patrick Roose, Udo A.Th. Brinkman, “Determination of volatile organic compounds in marine biota”Journal of Chromatography A 1998, 799,233-248
19. Wheat P.E., M.A. Tumeo,“Ultrasound induced aqueous polycyclic aromatic hydrocarbon reactivity”Ultrasonics Sonochemistry 1997,4 , 55-59
20. Anton Gáplovský, Jana Donovalová, Štefan Toma, Robert Kubinec,“Ultrasound effects on photochemical reactions, Part 1: photochemical reactions of ketones with alkenes”Ultrasonics Sonochemistry 1997,4 , 109-115
21. 林瑞聰,“惡臭污染防治”,環保資訊雜誌1993,第6期,PP.14~15。
22. 劉國棟,“VOC管制趨勢展望”,工業污染防治1993,第48期,PP15-31。
23. Aaron L. Theis, Adam J. Waldack, Susan M. Hansen, Michael A. Jeannot,“Headspace Solvent Microextraction”Anal. Chem. 2001,73, 5651-5654
24. Buchholz K. D. and J. Pawliszyn,“Determination of phenols by solid-phase microextraction and gas chromatographic analysis”Environ. Sci. Technol. 1993, 27, 2844.
25. Pawliszyn,“Solid phase microextraction with thermal desorption using fused silica optical fibers”Anal. Chem.1990, 62, 2145.
26. Application Note of Supelco, “Solid Phase Microexaction:Theory and Optimization of Conditions”, Bulletin 923, Supelco.
27. 黃敬德、謝有容,”固相微萃取技術之原理及其應用”,1998,Chemistry, Dec.
28. J.Pawliszyn,“Solid Phase Microextraction:Theory and Practice”,Wiley-Vch, Inc.( 1997)
29. J.Pawliszyn,“Application of Solid Phase Microextraction”,RS.C, Inc.(1999)
30. Application Note of Supelco, “SPME Application Guide”, Bulletin 925, Supelco.
31. David. W. Potter and J. Pawliszyn,“Rapid determination of polyaromatic hydrocarbons and polychlorinated biphenyls in water using solid-phase microextraction and GC/MS”Environ. Sci. Technol. 1994, 28, 298.
32. Homepage of Sigma-Aldrich Corporation, Supelco Group, “Product Information of SPME”, http://www.sigma-aldrich.com
33. M. Ligor and B. Buszewski, “Solid Phase Microextraction as a Method for Preparing Environmental Samples”, Journal of Environmental Studies 1997, Vol. 6, No. 5
34. R. Eisert and K. Levsen, “Review – Solid Phase Microexaction Coupled to Gas Chromatography : A New Method for the Analysis of Organics in Water”, Journal of Chromatography A 1996, 733,143-157.
35. J. L. Schnoor, “Environmental Modeling – Fate and Transport of Pollutants in Water, Air and soil”, John Wiley & Sons Inc. 1996, pp.42~51, 328-331.
36. C. Rivasseau and M. Caude, “Comparison of On-Line SPE-HPLC and SPME-GC for the Analysis of Microcontaminants in Water”, Chromatographia 1995, Vol.41, pp.462-470
37. Application Note of Supelco, “Optimizing SPME : Parameters to Control to Ensure Consistent Results”, Note 95, Supelco.
38. Z. Zhang and J. Pawliszyn, “Sampling Volatile Organic Compounds Using a Modified Solid Phase Microextraction Device” Journal of High Resolution Chromatography, 19,155-160
39. A. Saraullo, P. A. Martos and J. Pawliszyn, “Water Analysis by Solid Phase Microextraction Based on Physical Chemical Properties of the Coating”, Analytical Chemistry 1996, 69, pp.1992-1998 (1997)
40. 新竹科學工業園區管理局首頁,http://www.sipa.gov.tw
41. Homepage of Varian Instrument Corporation, “Automation of the SPME Devices”, http://www.varian.com
42. 陸志德,羅俊光,“高科技產業相關水體中揮發性有機物分析之研究”,國立清華大學碩士論文 (2000)
43. 許慧萍,羅俊光,“環境水體中揮發性有機化合物分析方法建立與驗證”,國立清華大學碩士論文 (2001)
44. Ashish Bhatnager and H. Mlchael Cheung,“Sonochemical Destruction of Chlorinated C1 and C2 Volatile Organic Compounds in Dilute Aqueous Solution” Environ. Sci. Technol. 1994,28 , 1481-1486
45. Carvalho L.R.F, S.R. Souza, B.S. Martinis, M. Korn,“Monitoring of the ultrasonic irradiation effect on the extraction of airborne particulate matter by ion chromatography”Analytica Chimica Acta 1995, 317 , 171-179
46. Wen Lai Huang, Kai Ming Liang, Shi Hua Cui, Shou Ren Gu,“Influene of ultrasonic vibration on the mesoporosity and surface fractal dimensions of resultant silica xerogels”Materials Research Bulletin 2001, 36 , 461-470
47. Maria S. Kuyukina, Irena B. Ivshina, Jim C. Philp, Nick Christofi, Sandra A. Dunbar, Marina I. Ritchkova,“Recovery of Rhodococcus biosurfactants using methyl tertiary-butyl ether extraction”Journal of Microbiological Methods, 2001, 46 , 149-156
48. Michael R. Hoffmann,“Kinetic and Mechanism of the Sonolytic Destruction of Methyl tert-Butyl Ether by Ultrasonic Irradiation in the Presence of Ozone” Environ. Sci. Technol. 1998,32 ,3194-3199
49. Inez Hua and Michael R. Hoffmann,“Optimization of Ultrasonic Irradiation as an Advanced Oxidation Technology” Environ. Sci. Technol. 1997,31 ,2237-2243
50. Joon-Wun Kang, Hui-Ming Hung, Angela Lin and Michael R. Hoffmann,“Sonolytic Destruction of Methyl tert-Butyl Ether by Ultrasonic Irradiation: The Role of O3 H2O2 Frequency and Power Density” Environ. Sci. Technol. 1999,33 , 3199-3205
51. Lingshuang Cai, Jun Xing, Li Dong, Caiying Wu,“Application of polyphenylmethylsiloxane coated fiber for solid-phase microextraction combined with microwave-assisted extraction for the determination of organochlorine pesticides in Chinese teas”Journal of Chromatography A 2003,1015 ,11-21
52. Sandra Babic, Mira Petrovic, Marija Kastelan-Macan,“Ultrasonic solvent extraction of pesticides from soil”Journal of Chromatography A 1998,823 ,3-9
53. Gokhan Savaroglu, Ertunc Aral,“Ultrasonic Velocity and Isentropic Compressibilities of the Ternary Mixture Benzene + Acetone + Chloroform and their Corresponding Binary Mixtures at 298.15K”Journal of Molecular Liquids 2003, 105 ,79-92
54. Lowri S. de Jager, Anthony R.J. Andrews,“Development of a screening method for cocaine and cocaine metabolites in urine using solvent microextraction in conjunction with gas chromatography”Journal of Chromatography A 2001,911 ,97-105
55. Elefteria Psillakis, Nicolas Kalogerakis,“Application of solvent microextraction to the analysis of nitroaromatic explosives in water samples”Journal of Chromatography A 2001 ,907 ,211-219
56. Guillard C., P. Theron, P. Pichat, C. Petrier,“Evaluation of 1-octanol degradation by photocatalysis and ultrasound using SPME” Water Research 2002,36 ,4263-4272
57. Gyorgy Szo llo si , Istvan Kun, Bela Torok, Mihaly Bartok, “Ultrasonics in chemoselective heterogeneous metal catalysis Sonochemical hydrogenation of unsaturated carbonyl compounds over platinum catalysts” Ultrasonics Sochemistry 2000 ,7 ,173-176
58. Pardue JH, Moe WM, McInnis D. Thibodeaux LJ, Valsaraj KT, Maciasz E, Van Heerden I, Korevec N, Yuan QZ. “Chemical and microbiological parameters in New Orleans floodwater following Hurricane Katrina.” Environ Sci Technol 2005;39:8591-99.
59. Parra M A, Gonzalez L, Elustondo D, Garrigo R, Santamaria J M, “Spatial and temporal trends of volatile organic compounds (VOC) in rural area of northern Spain.” Sci Total Environ 2006; 370:157-67.
60. Antoniou, C.V., Koukouraki, E.E. and Diamadopoulos, E. “Determination of chlorinated volatile organic compounds in water and municipal wastewater using headspace–solid phase microextraction–gas chromatography.” Journal of Chromatography A 2006 1132, 310-314.
61. Casas, V., Llompart, M., Garcia-Jares, C., Cela, R., and Dagnac, T. “Multivariate optimization of the factors influencing the solid-phase microextraction of pyrethroid pesticides in water.” Journal of Chromatography A 2006 1124, 148-156.
62. Cháfer-Pericás, C., Herráez-Hernández, R., and Campíns-Falcó, P. “In-tube solid-phase microextraction-capillary liquid chromatography as a solution for the screening analysis of organophosphorus pesticides in untreated environmental water samples.” Journal of Chromatography A 20071141, 10-21.
63. Chiu, K.H., Wu, B.Z., Chang, C.C., Sree, U., and Lo, J.G. “Distribution of Volatile Organic Compounds over a Semiconductor Industrial Park in Taiwan.” Environmental Science & Technology 2005 39, 973-983.
64. Diez, C., Sanz, J., and Camara, C. “Recent developments in solid-phase microextraction coatings and related techniques.” Journal of Chromatography A 2006, 1103, 183-192.
65. Merckel, C., Pragst, F., Ratzinger, A., Aebi, B., Bernhard, W., and Sporkert, F. “Application of headspace solid phase microextraction to qualitative and quantitative analysis of tobacco additives in cigarettes.” Journal of Chromatography A 2006, 1116, 10-19.
66. Ouyang, G.F. and Pawliszyn, J. “Recent developments in SPME for on-site analysis and monitoring.” Trends in Analytical Chemistry 2006, 25, 692-703.