Title

氣相層析同位素比質譜術區分高粱酒廠家及摻偽鑑定

Translated Titles

Discrimination of Manufacturers and Identification of Adulteration Kaoliang Liquor by Gas Chromatography/Isotope Ratio Mass Spectrometry

DOI

10.6843/NTHU.2013.00388

Authors

陳逸綸

Key Words

氣相層析 ; 同位素 ; 高粱酒 ; 廠家 ; 摻偽 ; 統計

PublicationName

清華大學化學系所學位論文

Volume or Term/Year and Month of Publication

2013年

Academic Degree Category

碩士

Advisor

凌永健

Content Language

繁體中文

Chinese Abstract

高粱酒在台灣是排名前三名產量的酒類,又以金門高粱最有名, 因此常有假冒的金門高粱在市面上流通,除了使用不實的標籤之外, 也可能添加食用香精或酒用香精,以增加酒中香氣或符合品質標準, 這些方式若只憑外觀、酒色、香氣等主觀的鑑定,沒有辦法輕易做出 正確辨識的。 本研究利用分散式液液微萃取進行前處理,結合氣相層析串聯同 位素比質譜儀,針對特定目標物進行 δ 13 C 分析,其優點在於物種的 固碳比例,並不會受到外來因素而產生變化,可以做為廠商判斷及區 域來源區別的依據。針對 34 瓶高粱酒分析之後,以 δ 13 C 的數據進行 統計分析,判別分析以乙醇、乙酸乙酯、己酸乙酯、2-苯乙醇、辛酸 乙酯、月桂酸乙酯及異戊醇鑑定,可達到 100%的廠家區分,包含了 金門高粱酒的廠家;擴大到製酒區域可以得到 90%以上的準確率,其 中金門高粱酒可以 100%區別。PLS-DA 統計分析,可以區分金門高粱 酒和其他區域的高粱酒;亦可區分金門地區的不同酒廠之高粱酒。 在 高粱酒原料的部分,利用物種 δ 13 C 計算求得小麥的比例,所有樣品 均落在一般小麥的使用比例範圍之內。香精添加的檢測實驗,以酯類 作為觀察依據,根據模擬添加以及真實樣品的結果進行判讀,判斷其 中一樣品有添加酒用香精的疑慮。最後我們參考財政部的公告和文獻報導,輔以本研究成果,提出 金門高粱酒的鑑定流程。

Topic Category 基礎與應用科學 > 化學
理學院 > 化學系所
Reference
  1. Vanderlinde, 'Geographic Origin of Southern Brazilian Wines by Carbon and
    連結:
  2. Oxygen Isotope Analyses', Rapid Commun Mass Spectrom, 24 (2010),
    連結:
  3. Food Chemistry, 50 (2002), 7520-23.
    連結:
  4. 3 R. M. Alonso-Salces, J. M. Moreno-Rojas, M. V. Holland, F. Reniero, C.
    連結:
  5. Stable Isotopes and Olive Oil Adulteration with Pomace Oil', Journal of
    連結:
  6. Agricultural and Food Chemistry, 45 (1997), 3044-48.
    連結:
  7. Preconcentration by Dispersive Liquid-Liquid Microextraction Procedure:
    連結:
  8. Recent Applications', Chromatographia, 74 (2011), 651-79.
    連結:
  9. Spectrometry Coupled to Liquid and Gas Chromatography for Wine Ethanol
    連結:
  10. Characterization', Rapid Commun Mass Spectrom, 22 (2008), 3111-8.
    連結:
  11. European Wine Glycerol: Stable Carbon Isotope Approach', Journal of
    連結:
  12. Agricultural and Food Chemistry, 52 (2004), 5902-06.
    連結:
  13. and J. Hoogewerff, 'Isotopic and Elemental Data for Tracing the Origin of
    連結:
  14. European Olive Oils', J Agric Food Chem, 58 (2010), 570-7.
    連結:
  15. 10 Federica Camin, Roberto Larcher, Matteo Perini, Luana Bontempo, Daniela
    連結:
  16. Bertoldi, Giacomo Gagliano, Giorgio Nicolini, and Giuseppe Versini,
    連結:
  17. 'Characterisation of Authentic Italian Extra-Virgin Olive Oils by Stable Isotope Ratios of C, O and H and Mineral Composition', Food Chemistry, 118
    連結:
  18. Spectrometry', Rapid Commun Mass Spectrom, 26 (2012), 1232-40.
    連結:
  19. 12 Luis F. Cuevas-Glory, Jorge A. Pino, Louis S. Santiago, and E. Sauri-Duch, 'A
    連結:
  20. Review of Volatile Analytical Methods for Determining the Botanical Origin
    連結:
  21. of Honey', Food Chemistry, 103 (2007), 1032-43.
    連結:
  22. 'Ionic Liquid Based Dispersive Liquid-Liquid Microextraction of Aromatic
    連結:
  23. Amines in Water Samples', Chinese Chemical Letters, 19 (2008), 985-87.
    連結:
  24. N. Yoshida, and G. S. Remaud, 'Comparison of Irms and Nmr Spectrometry
    連結:
  25. Oilseed Oils by Stable Carbon Isotope Analysis', Journal of the American Oil
    連結:
  26. Anal Bioanal Chem, 401 (2011), 1551-8.
    連結:
  27. Essential Oils Containing Linalool and Linalyl Acetate by Isotopic Methods',
    連結:
  28. Journal of Agricultural and Food Chemistry, 40 (1992), 81-87.
    連結:
  29. Yoshida, 'An Improved Method for the Measurement of the Isotope Ratio of
    連結:
  30. Beverages', Rapid Commun Mass Spectrom, 22 (2008), 3410-4.
    連結:
  31. 19 Jochen Jung, Tatjana Jaufmann, Uwe Hener, Andreas Münch, Mirjam Kreck,
    連結:
  32. Helmut Dietrich, and Armin Mosandl, 'Progress in Wine Authentication:
    連結:
  33. Implementation of Principal Component Analysis (Pca) for Classification
    連結:
  34. According to Geographical Origin', Food Chemistry, 73 (2001), 501-14.
    連結:
  35. Authenticity of Single Seed Vegetable Oils Using Fatty Acid Stable Carbon
    連結:
  36. Microextraction Method Based on Solidification of Floating Organic Drop
    連結:
  37. Combined with Gas Chromatography with Electron-Capture or Mass
    連結:
  38. Spectrometry Detection', Journal of Chromatography A, 1211 (2008), 8-12.
    連結:
  39. (Hsspme) for the Determination of Volatile and Semivolatile Pollutants in
    連結:
  40. Soils', Talanta, 48 (1999), 451-59.
    連結:
  41. 24 W. Meier-Augenstein, 'Applied Gas Chromatography Coupled to Isotope
    連結:
  42. Combination of Irms and Snif-Nmr Analyses', Journal of Agricultural and
    連結:
  43. Food Chemistry, 49 (2001), 1432-40.
    連結:
  44. Chromatography Combusiton-Isotope Ratio Mass Spectrometry', Food
    連結:
  45. 27 Ute Römisch, Henry Jäger, Xavier Capron, Silvia Lanteri, Michele Forina, and
    連結:
  46. Classification Methods', European Food Research and Technology, 230
    連結:
  47. (2009), 31-45.
    連結:
  48. 28 Y. H. Rau, G. P. Lin, W. S. Chang, S. S. Wen, and W. G. Fu, 'Using C-13/C-12
    連結:
  49. 29 Mohammad Rezaee, Yaghoub Assadi, Mohammad-Reza Milani Hosseinia,
    連結:
  50. Compounds in Water Using Dispersive Liquid-Liquid Microextraction',
    連結:
  51. Journal of Chromatography A, 1116 (2006), 1-9.
    連結:
  52. 30 C. Rhodes, K. Heaton, I. Goodall, and P. Brereton, 'Gas Chromatography Carbon Isotope Ratio Mass Spectrometry Applied to the Detection of
    連結:
  53. Chemistry, 114 (2009), 697-701.
    連結:
  54. of Rapeseed (Brassica Napus) Oils by Bulk C, O, H, and Fatty Acid C Stable
    連結:
  55. Isotope Analyses', J Agric Food Chem, 58 (2010), 8048-55.
    連結:
  56. Characterization of Olive Oils. I - Compositional and Carbon-13 Profiles of
    連結:
  57. 33 S. Wold, H. Martens, and H. Wold, 'The Multivariate Calibration Problem in
    連結:
  58. Chemistry Solved by the Pls Method', Lecture Notes in Mathematics, 973
    連結:
  59. (1983), 286-93.
    連結:
  60. Journal of Essential Oil Research, 23 (2011), 60-71.
    連結:
  61. Chromatography–Combustion-Isotope Ratio Mass Spectrometry
    連結:
  62. Kocsi, Roman Schoula, Francois Jaarsveld, and Reiner Wittkowski,
    連結:
  63. 'Characterisation and Determination of the Geographical Origin of Wines.
    連結:
  64. Part Ii: Descriptive and Inductive Univariate Statistics', European Food
    連結:
  65. Oil by Carbon Isotope Analysis of Individual Fatty Acids: Implications for
    連結:
  66. Authentication', Journal of Agricultural and Food Chemistry, 46 (1998),
    連結:
  67. 40 Madeleine E. Spitzke, and Carsten Fauhl-Hassek, 'Determination of the 13c/12c Ratios of Ethanol and Higher Alcohols in Wine by Gc-C-Irms
    連結:
  68. Analysis', European Food Research and Technology, 231 (2010), 247-57.
    連結:
  69. 41 S. Ulrich, 'Solid-Phase Microextraction in Biomedical Analysis', Journal of
    連結:
  70. Chromatography A, 902 (2000), 167-94.
    連結:
  71. 42 Z. Y. Zhang, and J. Pawliszyn, 'Headspace Solid-Phase Microextraction',
    連結:
  72. Analytical Chemistry, 65 (1993), 1843-52.
    連結:
  73. 43 林志鈞 張德明 謝建元 李秉真, '中式白酒成分、口感及消費者行為之分
    連結:
  74. 44 杜婷婷, ' 植物油微波輔助甲酯化方法建立及鑑定方法研究', 國立清華大
    連結:
  75. 48 袁玉潔, '氣相層析同位素比質譜儀及頂空氣相層析質譜儀鑑定酒類摻假
    連結:
  76. 50 郭中平 , 段國仁, '<利用液態發酵的方法進行高粱酒的釀造實驗及其香味之
    連結:
  77. 51 陳郁雯, '高粱酒成分分析與品牌鑑定', 國立清華大學 (2011).
    連結:
  78. 1 L. Adami, S. V. Dutra, A. R. Marcon, G. J. Carnieli, C. A. Roani, and R.
  79. 2943-8.
  80. 2 B. O. Aguilar-Cisneros, M. G. Lopez, E. Richling, F. Heckel, and P. Schreier,
  81. 'Tequila Authenticity Assessment by Headspace Spme-Hrgc-Irms Analysis of
  82. (13)C/(12)C and (18)O/(16)O Ratios of Ethanol', Journal of Agricultural and
  83. Guillou, and K. Heberger, 'Virgin Olive Oil Authentication by Multivariate
  84. Analyses of 1h Nmr Fingerprints and Delta13c and Delta2h Data', J Agric
  85. Food Chem, 58 (2010), 5586-96.
  86. 4 F. Angerosa, L. Camera, S. Cumitini, G. Gleixner, and F. Reniero, 'Carbon
  87. 5 Catalina Bosch Ojeda, and Fuensanta Sanchez Rojas, 'Separation and
  88. 6 L. Breiman, J. H. Friedman, R. A. Olshen, and C. G. Stone., 'Classification and
  89. Regression Trees.', Chapman and Hall (1984), 357.
  90. 7 A. I. Cabanero, J. L. Recio, and M. Ruperez, 'Isotope Ratio Mass
  91. 8 G. Calderone, N. Naulet, C. Guillou, and F. Reniero, 'Characterization of
  92. 9 F. Camin, R. Larcher, G. Nicolini, L. Bontempo, D. Bertoldi, M. Perini, C.
  93. Schlicht, A. Schellenberg, F. Thomas, K. Heinrich, S. Voerkelius, M. Horacek,
  94. H. Ueckermann, H. Froeschl, B. Wimmer, G. Heiss, M. Baxter, A. Rossmann,
  95. (2010), 901-09.
  96. 11 D. Chivall, R. Berstan, I. D. Bull, and R. P. Evershed, 'Isotope Effects
  97. Associated with the Preparation and Methylation of Fatty Acids by Boron
  98. Trifluoride in Methanol for Compound-Specific Stable Hydrogen Isotope
  99. Analysis Via Gas Chromatography/Thermal Conversion/Isotope Ratio Mass
  100. 13 Yun Chang Fan, Zheng Liang Hu, Mei Lan Chen, Chao Shen Tu, and Yan Zhu,
  101. 14 A. Gilbert, R. Hattori, V. Silvestre, N. Wasano, S. Akoka, S. Hirano, K. Yamada,
  102. for the Determination of Intramolecular 13c Isotope Composition:
  103. Application to Ethanol', Talanta, 99 (2012), 1035-9.
  104. 15 Lian-Xian Guo, Xiao-Ming Xu, Jian-Ping Yuan, Chou-Fei Wu, and Jiang-Hai
  105. Wang, 'Characterization and Authentication of Significant Chinese Edible
  106. Chemists' Society, 87 (2010), 839-48.
  107. 16 F. Guyon, L. Gaillard, M. H. Salagoity, and B. Medina, 'Intrinsic Ratios of
  108. Glucose, Fructose, Glycerol and Ethanol 13c/12c Isotopic Ratio Determined
  109. by Hplc-Co-Irms: Toward Determining Constants for Wine Authentication',
  110. 17 S. Hanneguelle, J. N. Thibault, N. Naulet, and G. J. Martin, 'Authentication of
  111. 18 R. Hattori, K. Yamada, K. Hasegawa, Y. Ishikawa, Y. Ito, Y. Sakamoto, and N.
  112. Ethanol in Various Samples, Including Alcoholic and Non-Alcoholic
  113. Gc–C/P–Irms Measurements of Glycerol and Gc Analysis of 2,3-Butanediol
  114. Stereoisomers', European Food Research and Technology, 223 (2006),
  115. 811-20.
  116. 20 S. Kallithraka, I. S. Arvanitoyannis, P. Kefalas, A. El-Zajouli, E. Soufleros, and E. Psarra, 'Instrumental and Sensory Analysis of Greek Wines;
  117. 21 S. Kelly, I. Parker, M. Sharman, J. Dennis, and I. Goodall, 'Assessing the
  118. Isotope Ratios (C-13/C-12)', Food Chemistry, 59 (1997), 181-86.
  119. 22 Mei- I. Leong, and Shang-Da Huang, 'Dispersive Liquid-Liquid
  120. 23 M. Llompart, K. Li, and M. Fingas, 'Headspace Solid Phase Microextraction
  121. Ratio Mass Spectrometry', Journal of Chromatography A, 842 (1999),
  122. 351-71.
  123. 25 N. Ogrinc, I. J. Kosir, M. Kocjancic, and J. Kidric, 'Determination of
  124. Authenticy, Regional Origin, and Vintage of Slovenian Wines Using a
  125. 26 I. G. Parker, S. D. Kelly, M. Sharman, M. J. Dennis, and D. Howie,
  126. 'Investigation into the Use of Carbon Isotope Ratios (C-13/C-12) of Scotch
  127. Whisky Congeners to Establish Brand Authenticity Using Gas
  128. Chemistry, 63 (1998), 423-28.
  129. Johanna Smeyers-Verbeke, 'Characterization and Determination of the
  130. Geographical Origin of Wines. Part Iii: Multivariate Discrimination and
  131. Isotopic Ratio Analysis to Differentiate between Rice Spirits Made from Rice
  132. and Cane Molasses', Journal of Food and Drug Analysis, 13 (2005), 159-62.
  133. Elham Aghaee, Fardin Ahmadi, and Sana Berijani, 'Determination of Organic
  134. Neutral Alcohol in Scotch Whisky: An Internal Reference Approach', Food
  135. 31 E. K. Richter, J. E. Spangenberg, M. Kreuzer, and F. Leiber, 'Characterization
  136. 32 A. Royer, C. Gerard, N. Naulet, M. Lees, and G. J. Martin, 'Stable Isotope
  137. Fatty Acids', Journal of the American Oil Chemists Society, 76 (1999), 357-63.
  138. 34 Luisa Schipilliti, Giovanni Dugo, Luca Santi, Paola Dugo, and Luigi Mondello,
  139. 'Authentication of Bergamot Essential Oil by Gas
  140. Chromatography-Combustion-Isotope Ratio Mass Spectrometer (Gc-C-Irms)',
  141. 35 Luisa Schipilliti, Paola Dugo, Ivana Bonaccorsi, and Luigi Mondello,
  142. 'Authenticity Control on Lemon Essential Oils Employing Gas
  143. (Gc–C-Irms)', Food Chemistry, 131 (2012), 1523-30.
  144. 36 Karin Schlesier, Carsten Fauhl-Hassek, Michele Forina, Valeriu Cotea, Emilia
  145. Part I: Overview', European Food Research and Technology, 230 (2009),
  146. 1-13.
  147. 37 Adnan Simsek, Mine Bilsel, and Ahmet C. Goren, '13c/12c Pattern of Honey
  148. from Turkey and Determination of Adulteration in Commercially Available
  149. Honey Samples Using Ea-Irms', Food Chemistry, 130 (2012), 1115-21.
  150. 38 Johanna Smeyers-Verbeke, Henry Jäger, Silvia Lanteri, Paul Brereton, Eric
  151. Jamin, Carsten Fauhl-Hassek, Michele Forina, and Ute Römisch,
  152. 'Characterization and Determination of the Geographical Origin of Wines.
  153. Research and Technology, 230 (2009), 15-29.
  154. 39 C. E. Spangenberg, S. A. Macko, and J. Hunziker, 'Characterization of Olive
  155. 4179-84.
  156. 析', Journal of Humanities and Social Sciences, Vol. 2, No. 2, pp. 25-35
  157. (2006).
  158. 學 (2011).
  159. 45 林書勳, '偽造金門高粱酒鑑識方法之研究:揮發性成分分析', 中央警察大
  160. 學 (2012).
  161. 46 金門酒廠, 'Http://Www.Kkl.Gov.Tw/'.
  162. 47 秦含章, '白酒釀造的科學與技術', 中國輕工業出版社 (1997).
  163. 之研究', 國立清華大學 (2009).
  164. 49 '財政部酒品認證標誌評審基準-高粱酒類(公告)'.
  165. 研究>', (2008).
  166. 52 陳順宇, '多變量分析'.
  167. 53 劉久年、劉仁驊, '飲酒的科學', 台北:渡假出版社 (1992).
  168. 54 歐陽港生, '中國傳統白酒香型與酒品', 中華民國酒業發展協進會會員通
  169. 訊, p 16 (1998).
  170. 55 蕭冬光, '白酒生產技術', 化學工業出版社 (2005).
  171. 56 薛聰賢, '台灣蔬果實用百科第二輯', 薛聰賢出版社 (2001).
Times Cited
  1. 歐怡君(2017)。消費者對於食品添加劑之看法及對清淨產品願付價格之研究-以豆乾為例。臺灣大學政治學研究所學位論文。2017。1-116。