Please use this identifier to cite or link to this item: http://hdl.handle.net/11455/3553
標題: 應答曲面實驗設計最適化超臨界二氧化碳萃取綠茶粉咖啡因製程
Response Surface Methodology to Optimize Supercritical Carbon Dioxide Extraction of Caffeine from Green Tea
作者: 黃國榮
Huang, Guo-Rong
關鍵字: Supercritical carbon dioxide;超臨界二氧化碳;co-solvent addition;caffeine;catechins;RSM;extraction efficiency;concentration factor;共溶劑添加;咖啡因;兒茶素;應答曲面實驗設計;去除率;濃縮因子
出版社: 化學工程學系所
引用: 參考文獻 1. 王重,史作清,施榮富和範雲鴿, “酚醛型吸附樹脂對咖啡因吸附效能的研究”, 高分子學報,第2卷,第211-215頁(2003)。 2. 何君慧, 蔣丙煌和余哲仁, “利用二氧化碳去除包種茶茶葉之咖啡因,” 國立台灣大學食品科技研究所碩士論文(2000) 。 3. 良邊文久, 衣笠仁和竹尾中一, “茶葉的簡易分離法,” 日本農藝化學會誌, Vol. 63(4), pp. 845-847 (1989) 。 4. 倪德江、陳玉瓊,「加工工藝對名優綠茶葉綠素變化的影響」,食品科學,第18卷,第12期,第14-18頁(1997)。 5. 胡熙恩,戴為智,王學軍,郭志俊,廖寶強和白潤生, “氯仿萃取咖啡因過程研究,” 清華大學學報,第3卷,第13-19頁(1995) 。 6. 郎慶勇,魏建謨,羅建苗和瞿港華, “臨界流體萃取技術的應用與展望,” 科儀新知,第20卷,第五期,第90-97頁(1999) 。 7. 莊志仁, “以超臨界二氧化碳萃取豬油中之膽固醇,” 國立台灣大學食品科技研究所碩士論文(1992) 。 8. 陳英玲, “茶葉的保健功效,” 科學發展,第391期,第66-73頁(2005) 。 9. 趙育漳, “包種茶湯之茶乳形成及其對膜濃縮加工之影響,” 國立台灣大學食品科技研究所博士論文(1994) 。 10. 黃業輝、陳曉陽、鄭弘發、曾貞,「兩類綠茶及其超微茶粉主要生化成分的研究」,茶葉通訊,第4期,第27-28頁(2002)。 11. 陸錦時、譚和平,「綠茶儲藏過程中主要品質化學成分的變化特點」,西南農業學報,第7卷,第77-81頁(1994)。 12. 戚向陽,謝筆鈞和胡慰望, “高純度表沒食子兒茶素沒食子酸酯(ECGC)的分離與製備,”精細化工, 第11卷,第40-46頁(1994)。 13. 張凱衣和肖純, “台灣綠茶加工簡介,”茶葉,第20卷,第2期,第41-42頁(1994) 。 14. 葉怡真, “樟芝對血管內皮細胞之影響及保心血管疾病之機制探討, ” 中國醫藥大學營養研究所碩士論文(2002) 。 15. 謝昌衛,“超臨界二氧化碳與界面活性劑包覆脂解提高鮪魚油中多元不飽和脂肪酸之研究,”中興大學食品科學研究所博士論文(2005)。 16. Ahmad, N. and Hasan, M., “Green Tea Polyphenols and Cancer: Biologic Mechanisms and Practical Implications,” Nutrition Reviews, Vol. 57, pp. 78-83 (1999). 17. Akagi, M., Fukuishi, N., Kan, T., Sagesaka, Y. M. and Akagi, R. “Anti-allergic Effect of Tea-Leaf Saponin (TLS) from Tea Leaves (Camellia sinensis var. sinensis),“ Biological Pharmaceutical Bulletin , Vol. 20, No. 5, pp. 565-567 (1997). 18. Apostolides, Z., Balentine, D.A., Harbowy, M.E., Hara, Y., and Weisburge, J.H., “Inhibition of PhIP Mutagenicity by Catechins, and by Theaflavins and Gallate Ester,” Mutation Research, Vol. 389, pp. 167-172. (1997). 19. Brunner, G. and Peter, S., “On the solubility of glycerides and fatty acid in the presence of an entrainer,”Separation Science and Technology , Vol. 17(1), pp. 199-203(1982). 20. Camy, S. and Condoret, J.S., “Dynamic modelling of a fractionation process for a liquid mixture using supercritical carbon dioxide,” Chemical Engineering and Processing, Vol.40, pp.499-509 (2001). 21. Catchpole, O.J., Grey, J.B., and Noermark, K.A., “Fractionation of fish oils using supercritical CO2 and CO2 ethanol mixtures,” Journal of Supercrit.l Fluids, Vol.19, pp.25-37 (2000). 22. Chiu, Y.W. and Tan, C.S., “Regeneration of Supercritical Carbon Dioxide by Membrane at Near Critical Conditions,” The Journal of Supercritical Fluidsn, Vol. 21, pp. 81-89 (2001). 23. Chang C.J., Chiu, K.L., Chen, Y.L., and Chang, C.Y., “Separation of Catechins from Green Tea Using Carbon Dioxide Extraction,” Food Chemistry, Vol. 68, pp. 109-113 (2000). 24. Chang C. J., Chiu, K.L., Chen, Y.L., Chang C.Y., and Yang, P.W., “Effect of Ethanol Content on Carbon Dioxide Extraction of Polyphenols from Tea,” Journal of Food Composition and Analysis, Vol. 14, pp. 75-82 (2001). 25. Chang, C.J., Randolph, A.D., and Craft, N.E., “Separation of β-carotene Mixtures Precipitated from Liquid Solvents with High Pressure CO2,” Biotechnology Progress, Vol.7, No.3, pp.275-278 (1991). 26. Chang, C.J. and Randolph, A.D. “Precipitation of microsize organic particles from supercritical fluids,” AIChE Journal, Vol.35, No.11, pp.1876-1882 (1989). 27. Chu, K.O., Wang, C.C., Chu, C.Y., Rogers, M.S., Choy, K.W., Pang, C.P., “Determination of Catechins and Catechin Gallates in Tissue by Liquid Chromatography with Coulometric Array Detection and Selective Solid Phase Extraction,” Journal of Chromatography B, Vol. 810, pp. 187-195 (2004). 28. Chung, L., Cheung, T., Kong, S., Fung, K., Choy, Y., Chan, Z., and Kwok, T., “Induction of Apotosis by Green Tea Catechins in Human Prostate Cancer DU145 cells,” Life Sciences, Vol. 68, pp. 1207-1214 (2001). 29. Ding, M., Yang, H., Xiao, S., “Rapid, Direct Determination of Polyphenols in Tea by Reverse-Phase column liquid chromatography,” Journal of Chromatography A, Vol. 849, pp. 637-640 (1999). 30. Garcia, A.A., Grange, B.C., Gandara, J.S., “Development of a Rapid Method Based on Solid-phase Extraction and Liquid Chromatography with Ultraviolet Absorbance Detection for the Determination of Polyphenols in Alcohol-free bees,” Journal of Chromatography Application, Vol. 1054, pp. 175-180, (2004). 31. Gast, K., Jungfer, M., Saure, C., and Brunner, G., “Purification of tocochromanols from edible oil,” Journal of Supercritical Fluids, Vol.34, pp.17-25 (2005). 32. Goto, T., Yoshida, Y., Kiso, M., and Nagashima, H., “Simultaneous Analysis of Individual Catechins and Caffeine in Green Tea.” Journal of Chromatography Applications, Vol. 749, pp. 295-299 (1996) 33. Graham, D.M. , “Caffeine-its Identity, Dietary Sources, Intake and Biological Effects,” Nutrition Reviews, 35(4):97,98 (1978). 34. Ham, A.J.L. and Liebler, D.C., “Antioxidant Reactions of Vitamin E in the Perfused Rat Liver: Product Distribution and Effect of Dietary Vitamin E Supplementation,” Archives of Biochemistry and Biophysics, Vol. 339, No.1, pp. 157-164 (1997). 35. Horvath, P.M. “Synergistic Effect of Vitamin E and Selenium in The Chemoprevention of Mammary Carcinogenesis in rats,” Cancer Research, Vol. 43, pp. 5335-5341 (1983). 36. Hung, Y.C., Sava, V.M., Makan, S.Y., Chen, T.H.J., Hong, M.Y., and Huang, G. S., “Antioxidant activity of Melanins Derived from Tea: Comparison Between Different Oxidative States,” Food Chemistry, Vol. 78, pp. 233-240 (2002). 37. Kimoto, T., Arai, S., Kohguchi, M., Aga, M., Nomura, Y., Micallef, M.J., Kurimoto, M., and Mito, K., “Apoptosis and Suppression of Tumor Growth by Artepillin C Extracted from Brazilian Propolis,” Cancer Detection and Prevention, Vol. 22, pp. 506-515 (1998). 38. Lea, M., Xiao, Q., Sadhukhan, A., Cottle, S., Wang, Z.Y., and Yang, C.S., “Inhibition Effects of Green Tea Extracts and (-)Epigallocatechin gallate on DNA Synthesis and Proliferation of Hepatoma and Erythroleukemia Cells,” Cancer Letters, Vol. 68, pp. 231-236 (1993). 39. Li, J. and Feng, Y.S., “A Study on Extraction of Tea polyphenols with Supercritical Carbon Dioxide,” Natural Product Research and Development, Vol. 8, pp. 42-47 (1996). 40. Li, P., Wang, Y., Ma, R., Zhang, X. “Separation of Tea polyphenols from Green Tea Leaves by A Combined CATUFM-adsorption Resin Process,” Journal of Food Engineering, Vol. 67, pp. 253-260 (2005). 41. Loro, J.F., del Rio, I., and Pérez-Santana, L., “Preliminary Studies of Analgesic and Anti-inflammatory Properties of Opuntia dillenii Aqueous Extract,” Journal of Ethnopharmacology, Vol. 67, pp. 213-218 (1999). 42. Mehr, C.B., Biswal, R.N. and Collins, J.L., “Supercritical Carbon Dioxide Extraction of Caffeine from Guarana,” The Journal of Supercritical Fluids, Vol. 9, pp. 185-191 (1996). 43. Mukhtar, H. and Nihal, A., “Green Tea in Chemoprevention of Cancer[Review],” The Journal of Toxicological Sciences, Vol. 52, pp. 111-117 (1999). 44. Nagalaksmi, S.,Jayalakshim, R. and Seshadri, R., “Approaches to Decreaming of Black Tea Diffusion by Solvent Decaffeination and Tannase Treatment,” International Journal of Food Science and Technology , Vol. 20, pp. 243-247 (1985). 45. No, J.K., Soung, D.Y., Kim, Y.J., and Shim, K.H., “Inhibition of Tyrosinase by Green Tea Components,” Pharmacology Letters, Vol. 65, pp. 241-246 (1999). 46. Ozawa, T., “Separation of the Components in Black Tea Infusion by Chromatography on Toyopearl®,” Agricultural Biological Chemistry, Vol. 46, No.4, pp. 1079-1081 (1982). 47. Palma, M. and Taylor, L.T., “Statistical Design for Optimization of Extraction of Polyphenols from An Inert Matrix Using Carbon Dioxide-based Fluids,” Analytica Chimica Acta, Vol. 391, pp. 321-329 (1999). 48. Papagiannopoulos, M. and Mellenthin, A. “Automated Sample Preparation by Pressurized Liquid Extraction-solid-phase Extraction for The Liquid Chromatography-mass Spectrometric Investigation of Polyphenols in the Brewing Process, “ Journal of Chromatography A, Vol. 976, pp. 345-348 (2002). 49. Park, H.S., Lee, H.J., and Shin, M.H. , “Decaffeination of green tea leaves using Supercritical Carbon Dioxide modified with a polar consolvent,” Food Chemical Toxicology. (2005). 50. Peker, H., Srinivasan, M.P., Smith, J.M. and Ben, J., “Caffeine Extraction Rates from Coffee Beans with Supercritical Carbon Dioxide,” AIChE Journal 38(5):761-763 (1992). 51. Pineiro, Z., Palma, M., and Barroso, C.G., “Determination of Catechins by Means of Extraction with Pressurized Liquid,” Journal of Chromatography A, Vol. 1026, pp. 19-23 (2004). 52. Qiu, Y., Chen, Y., Pei, Y., Matsuda, H., and Yoshikawa, M., “Constituents with Radical Scavenging Effect from Opuntia dillenii: Structures of New Alpha-pyrones and Flavonol Glycoside,” Chemical Pharmacentical Bulletin, Vol. 50, pp. 1507-1510 (2002). 53. Qiu, Y.K., Dou, D.Q., Pei, Y.P., Yoshikawa, M., Matsuda, H., and Chen, Y.J., “The Isolation and Identification of A New Alpha-pyrone from Opuntia dillenii,” Yao Xue Xue Bao., Vol. 38, pp. 523-525 (2003). 54. Rizvi, S.S.H., Danies, J.A., and Benado, A.L., “Supercritical fluid extraction: operation principles and food application,” Food Technology, Vol.6, pp.57-65 (1986). 55. Ryoyasu, S., ”Oxdiation and Chemical Structures of Two New Catechins from Fresh Tea Leaf,” Agricultural Biological Chemistry, Vol. 46, No.7, pp. 1969-1970 (1982). 56. Roy, P. and A.P. Kulkarni, “Oxidation of Ascorbic Acid by Lipoxygenase: Effect of Selected Chemicals,” Food Chemical Toxicology,Vol. 34, pp. 563-570 (1996) 57. Sato, T. and Miyata, G., “The Nutraceutical Benefit, Part 1: Green Tea,” Nutrition, Vol. 16, pp. 315-317 (2000). 58. Satoh, K., Sakamoto, Y., Ogata, A., Nagai, F., Mikuriya, H., Numazawa, M., Yamada, K., and Aoki, N., “Inhibition of Aromatase Activity by Green Tea Extract Catechins and Their Endocrinological Effects if Oral Administration in Rats,” Food and Chemical Toxicology, Vol. 40, pp. 925-933 (2002). 59. Segal, R. and Schlosser, E., “Role of Glycosidases in the Membranlytic, Antifungal Action of Saponins,” Archives of Microbiology , Vol. 104, pp. 147-150 (1975). 60. Shaw, P.E. and Buslig, B.S., “Selective Removal of Bitter Compounds from Grapefruit Juice and from Aqueous Solution with Cyclodextrin Polymer and with Amberlite XAD-4 ’ ,” Journal Agricultural Food Chemistry, Vol. 34, pp. 837-841 (1986). 61. Stahl, P., Quirin ,K.W. and Gerard ,D., “Dense gases for extraction and refining ,” Advances in Biochemical Engineering/Biotechnology ,p1 (1988). 62. Tatefuji, T., Izumi, N., Ohta, T., Arai, S., Ikeda, M., and Kurimoto, M., “Isolation and Identification of Compounds from Brazilian Propolis Which Enhance Macrophage Spreading and Mobility,” Biological Pharmacentical Bulletin, Vol. 19, pp. 966-970 (1996). 63. Tsuchiya, H., Sato, M., Kato, H., Kureshiro, H., Takagi, N., “Nanoscale Analysis of Pharmacologically Active Catechins in Body Fluid by HPLC Using Borate Complex Extraction Preferment,” Talanta, Vol. 48, pp.717-726, (1998). 64. Uesato, S., Kitagawa, Y., Kamishimoto, M., Kumagai, A., Hori, H., and Nagasawa, H., “Inhibition of Green Tea Catechins Against the Growth and Induction of Apoptosis in Human Colon and Hepatic Epothelial Cells,” Cancer Letter, Vol. 170, pp. 41-44 (2001). 65. Uemura, T., Sagesaka, Y. M., Oku, N. and Okada, S., “Activation of Retinoic acid (RA)-differentiated HL-60 cells by saponins,” Yakugaku Zasshi (in Japanese), Vol. 115, pp. 528-536 (1995). 66. Vogel,G., Marek, M.L., and Oertner, R., “Pharmacology of the Saponin of Tea Seeds, a Saponin MIture of Thea Sinensis L.,” Arzneimittel Forschung (in German), Vol. 18, pp. 1466-1467 (1968). 67. Wang, H., Helliwell, K., You, X., “Isocratic elution system for the Determination of Catechins, Caffieine and Gallic Acid in Green Tea Using HPLC,” Food Chemistry, Vol. 68, pp. 115-121, (2000). 68. Yokozawa, T., Chen, C.P., Dong, E., Tanaka, T., Nonaka, G., and Nishiok, I., “Study on the Inhibitory Effect of Tannins and Flavonoids Against the 1,1-Diphenyl-2-Picryhydrazyl Radical,” Biochemical Pharmacology, Vol. 56, pp. 213-222 (1998). 69. Yoshida, Y., Kiso, M., and Goto, T., “Efficiency of The Extraction of Catechins from Green Tea,” Food Chemistry, Vol. 67, pp. 429-433 (1999). 70. Yu, E.K.C., “Novol Decaffeination Process Using Cyclodextrins,” Applied Microbiology and Biotechnology, Vol. 25, pp. 546-548 (1988). 71. Zosel, A., “Process for the Decaffeination from Coffee,”U.S.patent, pp.4,260,239 (1981). 72. Zuo, Y., Chen, H., and Deng, Y., “Simultaneous Determination of Catechins, Caffeine and Gallic Acids in Green, Block and Pu-erh Teas Using HPLC with a Photodiode Array Detector,” Talanta, Vol. 57, pp. 307-316 (2002).
摘要: 
本研究探討添加共溶劑之超臨界二氧化碳,去除綠茶茶粉中之咖啡因的最適條件。以應答曲面實驗設計法,找出添加水之超臨界二氧化碳的萃取條件,對咖啡因去除率(RCAF)、兒茶素萃出率(RCAT)、咖啡因濃縮倍數(βCAF)、兒茶素濃縮倍數(βCAT)及咖啡因去除率與兒茶素保留率乘積值(RCAF) (100-RCAT)的應答曲面關係。
1克水潤濕4克 74μm茶粉30分鐘後,以12 mL/min 、3600克的二氧化碳,萃取14小時,在333K、300bar萃取,可去除茶葉中95.6%之咖啡因,且兒茶素之保留率有80.2%。如降低茶粉粒徑至74μm時,在333K,300bar,添加7克水(2克預添加、5克連續添加)之800克超臨界二氧化碳,萃取1.7小時,咖啡因去除率可達100%。應答曲面分析預測,如考慮咖啡因去除率與兒茶素保留率時,在323K,275bar,添加6克水(2克預添加、4克連續添加)之640克超臨界二氧化碳,萃取8克74μm茶粉1.2小時,將得71.9 %咖啡因去除率與67.3%兒茶素保留率。結果顯示,水修飾的超臨界二氧化碳,雖能大幅減少二氧化碳使用量與萃取時間,但相對地無法避免兒茶素被萃出的損失量。

This work studied co-solvent modified supercritical carbon dioxide (SC-CO2) to remove caffeine from green tea. Response Surface Methodology (RSM) was employed to determine operation conditions with respect to the caffeine extraction efficiency (RCAF), the catechins extraction efficiency (RCAT), the concentration factor of caffeine (βCAF), the concentration factor of catechins (βCAT) and the product of (RCAF) (100-RCAT).
Experimental data indicated 95.6% caffeine was removed and 80.2% catechins was remained by 3600 gram SC-CO2 at 333K and 300bar extraction of 4 gram 74μm tea powder wetted by 1 gram water.Continuously adding water modified 800 gram SC-CO2 extracted at 333K and 300bar, removed 100% caffeine from 8 gram green tea. The study of Response Surface Methodology presseated that 640 gram SC-CO2 that extraced of 8 gram green tea at the 313K and 200bar condition removed 71.9% caffeine and still retained 67.3% Catechins.
URI: http://hdl.handle.net/11455/3553
其他識別: U0005-0602200718114300
Appears in Collections:化學工程學系所

Show full item record
 

Google ScholarTM

Check


Items in DSpace are protected by copyright, with all rights reserved, unless otherwise indicated.