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研究生: 徐子欣
Hsu, Tzu-Hsin
論文名稱: 微型氣相層析儀應用於呼氣丙酮及中草藥材氣味分析之研究
The Applications of Micro-GC on Breath Acetone and Herbal Medicine Scent Analysis
指導教授: 呂家榮
Lu, Chia-Jung
口試委員: 周芳妃 宋蕙伶
口試日期: 2021/05/26
學位類別: 碩士
Master
系所名稱: 化學系
Department of Chemistry
論文出版年: 2021
畢業學年度: 109
語文別: 中文
論文頁數: 96
中文關鍵詞: 呼氣丙酮非侵入式檢測中草藥材氣味微型氣相層析儀
英文關鍵詞: breath acetone, non-invasive, Micro-GC, scent of herbal medicine
研究方法: 實驗設計法
DOI URL: http://doi.org/10.6345/NTNU202100747
論文種類: 學術論文
相關次數: 點閱:81下載:4
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  • 糖尿病是 全世界 近幾年來非常盛行的慢性文明病,目前也有學者正研究人體呼出的有機揮發性氣 體 (VOCs)所帶給人體生理上的反應,以及利用非侵入式的方法檢測人體 。 另外, 近年來中草藥材中所散發出的氣味 是否正確 也成為人們生活上的一項課題,相同的中草 藥材卻散發出不同的 香氣 ,目前有許多研究與電子鼻相關,模擬了人體的嗅覺模式去進行不同物種的比對。本論文主要以人體呼出 的 有機揮發物以及中草藥材 氣味化合物這兩項為研究主題,人體呼氣的受試者招募了 共 12位 糖尿病患者以及 生理健康人體, 利用本實驗室自製的 氣體採集袋 進行呼氣檢測,而中藥材氣味找尋了杜仲的傳統中草藥材和科學中藥,模擬頂空 的方式採集中草藥材上方的氣體進行研究利用氣相層析質譜儀和本實驗室開發的微型氣相層析儀 進行分析 。本論文研究出了糖尿病患者與呼氣丙酮濃度的相關,以及人體呼氣出的有機揮發物 反應了人體一定的代謝狀態,也探討相同中草藥材於不同產地採收所散發出氣味化合物的異同,和複方科學中藥透過單方科學中藥混合時,所散發出的氣味和濃度是否有加成性 ,並以微型氣相層析儀取代電子鼻,使數據有更高的精確度。

    Diabetes is a chronic disease that is very prevalent all over the world in recent years. At present, some scholars are studying the physiological response of the human body's exhaled Organic Volatile Compounds (VOCs), and the use of non-invasive methods to detect the human body's breath. In addition, in recent years, whether the smell emitted by herbal medicine is correct has also become a topic in our life. The same herbal medicine emits different aromas. At present, there are many studies related to Electronic-noses that simulate the human body’s olfactory pattern to perform different scents and comparison of species.
    The thesis mainly focuses on the two research topics of human body exhaled Organic Volatiles Compounds and herbal medicine compounds. The human exhalation subjects recruited a total of 12 diabetic patients and physically healthy human bodies, and used the self-made gas collection bag in our laboratory to exhale. Detection the smell of herbal medicine searched for herbal medicine materials and scientific herbal medicine of Eucommia ulmoides. The gas above the herbal medicine materials was collected by Headspace (HS). The gas chromatography mass spectrometry and the micro-gas chromatography developed in our laboratory were used for analysis.

    目錄 摘要 I Abstract II 目錄 III 表目錄 VI 圖目錄 VII 第一章 緒論 1 1.1 前言 1 1.2 人體呼氣作用和其所在環境 5 1.3 呼氣中有機揮發物反應之疾病 7 1.3.1 糖尿病與丙酮 7 1.3.2 膽固醇與異戊二烯 9 1.4 電子鼻應用 11 1.5 中草藥氣味 13 1.5.1 杜仲 14 1.5.2 三黃瀉心湯 15 1.5.2.1大黃 16 1.5.2.2黃連 16 1.5.2.3黃芩 17 1.6 人體呼氣揮發性有機物採集方式 18 1.7 中草藥材氣味分析採集方式 19 第二章 實驗部分 20 2.1 實驗藥品與器材 20 2.1.1 實驗藥品 20 2.1.2 實驗儀器與器材 22 2.2 前濃縮系統 23 2.2.1 前濃縮系統介紹 23 2.2.2 六向閥狀態 24 2.2.3 前濃縮管系統與使用流程 27 2.3 氣相層析質譜儀 31 2.4 微型氣相層析儀 32 2.5 樣品採樣方式 33 2.5.1 呼氣中揮發性有機物 33 2.5.2 中草藥材氣味化合物 35 第三章 結果與討論 37 3.1 採樣參數 37 3.1.1 Tedlar採氣袋與自製採氣袋 37 3.1.2 採氣袋回收率 39 3.1.3 氣體來源 42 3.2 呼氣揮發性有機物 42 3.2.1 呼氣中的丙酮 44 3.2.2 呼氣中的異戊二烯 45 3.3 單方中藥材-杜仲 47 3.3.1 台北市與台中市某中草藥材行 49 3.3.2 三間不同廠牌之杜仲科學中藥 60 3.4 複方中藥材-三黃瀉心湯 67 3.5 微型氣相層析儀應用於中草藥材氣味 70 3.5.1 台北市與台中市某中草藥材行 70 3.5.2 三間不同廠牌之杜仲科學中藥 73 3.5.3 複方中藥材-三黃瀉心湯 75 第四章 結論 77 附錄 80 參考文獻 91

    1. Haynes, W. M.; Lide, D. R.; Bruno, T. J., CRC Handbook of chemistry and physics. 2017.
    2. Homaira, N.; Jaffe, A., Pleural Effusion, Necrotizing Pneumonia and Long-Term Morbidity of Respiratory Infection in Childhood. In Reference Module in Biomed. Sci., Elsevier: 2021.
    3. Ruzsányi, V.; Péter Kalapos, M., Breath acetone as a potential marker in clinical practice. J. Breath Res. 2017, 11 (2), 024002.
    4. Watelet, J. B.; Katotomichelakis, M.; Eloy, P.; Danielidis, V., The physiological basics of the olfactory neuro-epithelium. B-ent. 2009, 5 Suppl. 13, 11-9.
    5. Persaud, K.; Dodd, G., Analysis of discrimination mechanisms in the mammalian olfactory system using a model nose. Nature 1982, 299 (5881), 352-5.
    6. Deng, C.; Liu, N.; Gao, M.; Zhang, X., Recent developments in sample preparation techniques for chromatography analysis of traditional Chinese medicines. J. Chromatogr A 2007, 1153 (1-2), 90-6.
    7. Winterstein, H., Chemical regulation of respiration. Ergeb Physiol. 1955, 48, 328-528.
    8. Stolz, C., The 1st breath. Anaesthesist 1970, 19 (12), 449-57.
    9. Mortola, J. P., How to breathe? Respiratory mechanics and breathing pattern. Respir Physiol. Neurobiol. 2019, 261, 48-54.
    10. Nguyen, T.-A.; Woo-Park, J.; Hess, M.; Goins, M.; Urban, P.; Vaughan, J.; Smith, A.; Hunt, J., Assaying all of the nitrogen oxides in breath modifies the interpretation of exhaled nitric oxide. Vascul. Pharmacol. 2005, 43 (6), 379-384.
    11. Vasilescu, A.; Hrinczenko, B.; Swain, G. M.; Peteu, S. F., Exhaled breath biomarker sensing. Biosens. Bioelectron. 2021, 182, 113193.
    12. Hibbard, T.; Killard, A. J., Breath Ammonia Analysis: Clinical Application and Measurement. Crit. Rev. Anal. Chem. 2011, 41 (1), 21-35.
    13. Wang, Z.; Wang, C., Is breath acetone a biomarker of diabetes? A historical review on breath acetone measurements. J. Breath Res. 2013, 7 (3), 037109.
    14. Sanchez, J. M., Air and breath analysis for the assessment of exposure to solvent emissions in university chemistry laboratories. Atmospheric Pollut. Res. 2019, 10 (6), 1795-1802.
    15. Chuang, M.-Y.; Lin, Y.-T.; Tung, T.-W.; Chang, L.-Y.; Zan, H.-W.; Meng, H.-F.; Lu, C.-J.; Tao, Y.-T., Room-temperature-operated organic-based acetone gas sensor for breath analysis. Sens. Actuators B Chem. 2018, 260, 593-600.
    16. Yang, T.; Gao, D. X.; Yu, Y. L.; Chen, M. L.; Wang, J. H., Dielectric barrier discharge micro-plasma emission spectrometry for the detection of acetone in exhaled breath. Talanta 2016, 146, 603-8.
    17. Königstein, K.; Abegg, S.; Schorn, A. N.; Weber, I. C.; Derron, N.; Krebs, A.; Gerber, P. A.; Schmidt-Trucksäss, A.; Güntner, A. T., Breath acetone change during aerobic exercise is moderated by cardiorespiratory fitness. J. Breath Res. 2020, 15 (1), 016006.
    18. Yokokawa, T.; Ichijo, Y.; Houtsuki, Y.; Matsumoto, Y.; Oikawa, M.; Yoshihisa, A.; Sugimoto, K.; Nakazato, K.; Suzuki, H.; Saitoh, S. I.; Shimouchi, A.; Takeishi, Y., Change of Exhaled Acetone Concentration in a Diabetic Patient with Acute Decompensated Heart Failure. Int. Heart J. 2017, 58 (5), 828-830.
    19. Li, Q.; Li, J.; Wei, X.; Li, Y.; Sun, M., An exploratory study on online quantification of isoprene in human breath using cavity ringdown spectroscopy in the ultraviolet. Ana.l Chim. Acta. 2020, 1131, 18-24.
    20. Sukul, P.; Richter, A.; Schubert, J. K.; Miekisch, W., Deficiency and absence of endogenous isoprene in adults, disqualified its putative origin. Heliyon 2021, 7 (1), e05922.
    21. Salerno-Kennedy, R.; Cashman, K. D., Potential applications of breath isoprene as a biomarker in modern medicine: a concise overview. Wien. Klin. Wochenschr 2005, 117 (5-6), 180-6.
    22. Stone, B. G.; Besse, T. J.; Duane, W. C.; Evans, C. D.; DeMaster, E. G., Effect of regulating cholesterol biosynthesis on breath isoprene excretion in men. Lipids 1993, 28 (8), 705-8.
    23. Karl, T.; Prazeller, P.; Mayr, D.; Jordan, A.; Rieder, J.; Fall, R.; Lindinger, W., Human breath isoprene and its relation to blood cholesterol levels: new measurements and modeling. J. Appl. Physiol. 2001, 91 (2), 762-70. 24. Cailleux, A.; Allain, P., Isoprene and sleep. Life Sci. 1989, 44 (24), 1877-1880.
    25. Euler, D. E.; Davé, S. J.; Guo, H., Effect of cigarette smoking on pentane excretion in alveolar breath. Clin. Chem. 1996, 42 (2), 303-308.
    26. Grabe, V.; Sachse, S., Fundamental principles of the olfactory code.Biosystems 2018, 164, 94-101.
    27. Zhou, Q.; Liu, S.; Liu, Y.; Song, H., Comparison of flavour fingerprint, electronic nose and multivariate analysis for discrimination of extra virgin olive oils. R. Soc. Open Sci. 2019, 6 (3), 190002.
    28. Haddi, Z.; Mabrouk, S.; Bougrini, M.; Tahri, K.; Sghaier, K.; Barhoumi, H.; El Bari, N.; Maaref, A.; Jaffrezic-Renault, N.; Bouchikhi, B., E-Nose and e-Tongue combination for improved recognition of fruit juice samples. Food Chem. 2014, 150, 246-53.
    29. Aouadi, B.; Zaukuu, J. Z.; Vitális, F.; Bodor, Z.; Fehér, O.; Gillay, Z.; Bazar, G.; Kovacs, Z., Historical Evolution and Food Control Achievements of Near Infrared Spectroscopy, Electronic Nose, and Electronic Tongue-Critical Overview. Sensors (Basel) 2020, 20 (19).
    30. Rocco, R.; Incalzi, R. A.; Pennazza, G.; Santonico, M.; Pedone, C.; Bartoli, I. R.; Vernile, C.; Mangiameli, G.; La Rocca, A.; De Luca, G.; Rocco, G.; Crucitti, P., BIONOTE e-nose technology may reduce false positives in lung cancer screening programmes†. Eur. J. Cardiothorac Surg. 2016, 49 (4), 1112-7.
    31. Thaler, E. R.; Huang, D.; Giebeig, L.; Palmer, J.; Lee, D.; Hanson, C. W.; Cohen, N., Use of an electronic nose for detection of biofilms. Am. J. Rhinol. 2008, 22 (1), 29-33.
    32. Behera, B.; Joshi, R.; Anil Vishnu, G. K.; Bhalerao, S.; Pandya, H. J., Electronic nose: a non-invasive technology for breath analysis of diabetes and lung cancer patients. J. Breath Res. 2019, 13 (2), 024001.
    33. Popov, T. A., Human exhaled breath analysis. Ann. Allergy Asthma Immunol. 2011, 106 (6), 451-6.
    34. 張鐵軍 ;劉昌孝 ,中藥五味藥性理論辨識及其化學生物學實質表征路徑 .中草
    藥 Chinese Traditional and Herbal Drugs 2015, 46 (1), 1-6.
    35. 煌 ,曹 .;張鐵軍 ;張靜雅 ;龔蘇曉 ;浚 ,許 .;劉昌孝 , 基於電子鼻和電子舌技術的辛
    味中藥氣 -味的表徵研究 .中草藥 Chinese Traditional and Herbal Drugs 2016, 47 (11), 1962-1967.
    36. Wang, C. Y.; Tang, L.; He, J. W.; Li, J.; Wang, Y. Z., Ethnobotany, Phytochemistry and Pharmacological Properties of Eucommia ulmoides: A Review. Am. J. Chin. Med. 2019, 47 (2), 259-300.
    37. Liu, C.; Guo, F. F.; Xiao, J. P.; Wei, J. Y.; Tang, L. Y.; Yang, H. J., Research advances in chemical constituents and pharmacological activities of different parts of Eucommia ulmoides. Zhongguo Zhong Yao Za Zhi 2020, 45 (3), 497-512.
    38. He, X.; Wang, J.; Li, M.; Hao, D.; Yang, Y.; Zhang, C.; He, R.; Tao,R., Eucommia ulmoides Oliv.: ethnopharmacology, phytochemistry and pharmacology of an important traditional Chinese medicine. J. Ethnopharmacol 2014, 151 (1), 78-92.
    39. Zhu, M. Q.; Sun, R. C., Eucommia ulmoides Oliver: A Potential Feedstock for Bioactive Products. J. Agric. Food. Chem. 2018, 66 (22), 5433-5438.
    40. Zhang, W.; Li, F.; Gao, W., Tripterygium wilfordii Inhibiting Angiogenesis for Rheumatoid Arthritis Treatment. J. Natl. Med. Assoc. 2017, 109 (2), 142-148.
    41. Appiah, S.; Revitt, M.; Jones, H.; Vu, M.; Simmonds, M.; Bell, C., Antiinflammatory and Hepatoprotective Medicinal Herbs as Potential Substitutes for Bear Bile. Int. Rev. Neurobiol 2017, 135, 149-180.
    42. Li, C.-Y.; Hou, Y.-C.; Lee Chao, P.-D.; Shia, C.-S.; Hsu, I. C.; Fang, S.-H., Potential ex vivo immunomodulatory effects of San-Huang-Xie-Xin-Tang and its component herbs on mice and humans. J. Ethnopharmacol.2010, 127 (2), 292-298.
    43. Liu, C. Z.; Chen, D. W., Sanhuang tablets research. Zhongguo Zhong Yao Za Zhi 2007, 32 (17), 1827-9.
    44. Li, Y.; Xu, X., The content condition of effective composition in Sanhuang Xiexin decoction. Zhongguo Zhong Yao Za Zhi 2006, 31 (5), 383-5.
    45. Chen, Q. Y.; Fu, C. M.; Luo, R. F.; Lin, M. S.; Liao, W.; Gao, F., Research progress of effect of Rhei Radix et Rhizoma and its anthraquinone in treatment of autoimmune diseases. Zhongguo Zhong Yao Za Zhi 2021, 46 (1), 15-23.
    46. Wang, N.; Feng, Y.; Tan, H.-Y.; Cheung, F.; Hong, M.; Lao, L.; Nagamatsu, T., Inhibition of eukaryotic elongation factor-2 confers to tumor suppression by a herbal formulation Huanglian-Jiedu decoction in human hepatocellular carcinoma. J. Ethnopharmacol. 2015, 164, 309-318.
    47. Han, L.; Wang, R.; Zhang, X.; Yu, X.; Zhou, L.; Song, T.; Deng, X.; Zhang, Y.; Zhang, L.; Bai, C., Advances in Processing and Quality Control of Traditional Chinese Medicine Coptidis rhizoma (Huanglian): A Review. J. AOAC Int. 2019, 102 (3), 699-707.
    48. Yu-Min, F.; Meng-Ying, C.; Jie, L.; Tian-Lin, P.; Yu-Kun, W.; Qing, Z., Study advance in biosynthesis of flavone from Scutellaria. Zhongguo Zhong Yao Za Zhi 2020, 45 (20), 4819-4826.
    49. Shang, X.; He, X.; He, X.; Li, M.; Zhang, R.; Fan, P.; Zhang, Q.; Jia,Z., The genus Scutellaria an ethnopharmacological and phytochemical review. J. Ethnopharmacol. 2010, 128 (2), 279-313.
    50. Jian, R.-S.; Huang, Y.-S.; Lai, S.-L.; Sung, L.-Y.; Lu, C.-J., Compact instrumentation of a μ-GC for real time analysis of sub-ppb VOC mixtures. Microchem. J. 2013, 108, 161-167.
    51. Jian, R.-S.; Wang, T.-Y.; Song, L.-Y.; Kuo, C.-Y.; Tian, W.-C.; Lo, E.-W.; Lu, C.-J., Field investigations and dynamic measurements of process activity induced VOCs inside a semiconductor cleanroom. Build. Environ. 2015, 94, 287-295.
    52. Lawal, O.; Ahmed, W. M.; Nijsen, T. M. E.; Goodacre, R.; Fowler, S. J., Exhaled breath analysis: a review of 'breath-taking' methods for off-line analysis. Metabolomics 2017, 13 (10), 110.
    53. Martin, A. N.; Farquar, G. R.; Jones, A. D.; Frank, M., Human breath analysis: methods for sample collection and reduction of localized background effects. Anal. Bioanal. Chem. 2010, 396 (2), 739-50.
    54. Teng, Z. Q.; Hao, Q. X.; Jin, Y.; Guo, L. P., Comparison of volatile components in Schisandra propinqua from different habitats by HS-SPME-GC-MS. Zhongguo Zhong Yao Za Zhi 2018, 43 (15), 3216-3222.
    55. Nie, J.; Teng, Y.-J.; Li, Z.-G.; Liu, W.-H.; Lee, M.-R., Magnetic nanoparticles used in headspace extraction coupled with DSI-GC-IT/MS for analysis of VOCs in dry Traditional Chinese Medicine. Chin. Chem. Lett. 2016, 27 (1), 178-184.
    56. Gao, C.; Li, Y.; Pan, Q.; Fan, M.; Wang, L.; Qian, H., Analysis of the key aroma volatile compounds in rice bran during storage and processing via HS-SPME GC/MS. J. Cereal. Sci. 2021, 99, 103178.
    57. Lu, C. J.; Zellers, E. T., Multi-adsorbent preconcentration/focusing module for portable-GC/microsensor-array analysis of complex vapor mixtures. Analyst 2002, 127 (8), 1061-8.
    58. Beauchamp, J.; Herbig, J.; Gutmann, R.; Hansel, A., On the use of Tedlar® bags for breath-gas sampling and analysis. J. Breath Res. 2008, 2 (4), 046001.
    59. Phillips, M.; Cataneo, R. N.; Cheema, T.; Greenberg, J., Increased breath biomarkers of oxidative stress in diabetes mellitus. Clin. Chim. Acta 2004, 344 (1), 189-194.
    60. Tovbin, Y. K., Lattice-gas model in equilibrium, kinetic and dynamic problems of adsorption. Appl. Surf. Sci. 2002, 196 (1), 71-80.
    61. Rydosz, A., A Negative Correlation Between Blood Glucose andAcetone Measured in Healthy and Type 1 Diabetes Mellitus Patient Breath. J. Diabetes Sci. Technol. 2015, 9 (4), 881-4.
    62. Kanikarla-Marie, P.; Jain, S. K., Hyperketonemia and ketosis increase the risk of complications in type 1 diabetes. Free Radic. Biol. Med. 2016, 95, 268-77.
    63. Kushch, I.; Arendacká, B.; Stolc, S.; Mochalski, P.; Filipiak, W.; Schwarz, K.; Schwentner, L.; Schmid, A.; Dzien, A.; Lechleitner, M.; Witkovský, V.; Miekisch, W.; Schubert, J.; Unterkofler, K.; Amann, A., Breath isoprene--aspects of normal physiology related to age, gender and cholesterol profile as determined in a proton transfer reaction mass spectrometry study. Clin. Chem. Lab. Med. 2008, 46 (7), 1011-8.
    64. Brown, A. J.; Sharpe, L. J., Chapter 11 - Cholesterol Synthesis. In Biochemistry of Lipids, Lipoproteins and Membranes (Sixth Edition), Ridgway, N. D.; McLeod, R. S., Eds. Elsevier: Boston, 2016; pp 327-358.
    65. Król, S.; Zabiegała, B.; Namieśnik, J., Monitoring VOCs in atmospheric air I. On-line gas analyzers. Trends Analyt. Chem. 2010, 29 (9), 1092-1100.
    66. 華會明 ;尹宏權 ;李寶強 ; 裴月湖 , 杜仲化學成分的研究 .分子植物育種 2003, 1卷 5&6期 , P801 - 803.
    67. Kalász, H.; Antal, I., Drug excipients. Curr. Med. Chem. 2006, 13 (21), 2535-63.
    68. Abrantes, C. G.; Duarte, D.; Reis, C. P., An Overview of Pharmaceutical Excipients: Safe or Not Safe? J. Pharm. Sci. 2016, 105 (7), 2019-26.
    69. Zhang, H.; Chen, Y.; Wang, J. N.; Jiang, H. J.; Shen, X. W.; Yan, J. Z., Application of fingerprint technology in quality evaluation and process control of traditional Chinese medicine formula granules. Zhongguo Zhong Yao Za Zhi 2018, 43 (19), 3822-3827.
    70. Mo, Y. J.; Wang, Y.; Qi, Q.; Yu, X. L.; Luo, J. Y.; Hu, H. Y.; Liu, F.; Wu, J. X.; Lu, Y.; Du, S. Y.; Bai, J.; Li, P. Y., HPLC fingerprint of famous traditional formula Sanpian Decoction and quality value transmitting of Chuanxiong Rhizoma. Zhongguo Zhong Yao Za Zhi 2020, 45 (3), 572-578.

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