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http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/48223完整後設資料紀錄
| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 陳玉如(Yu-Ju Chen) | |
| dc.contributor.author | Tzu-Hsin Chan | en |
| dc.contributor.author | 詹子欣 | zh_TW |
| dc.date.accessioned | 2021-06-15T06:49:23Z | - |
| dc.date.available | 2013-07-06 | |
| dc.date.copyright | 2011-07-06 | |
| dc.date.issued | 2011 | |
| dc.date.submitted | 2011-03-16 | |
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(2004) Various nondigestible saccharides open a paracellular calcium transport pathway with the induction of intracellular calcium signalling in human intestinal Caco-2 cells, Journal of Nutrition 134, 1935-1941. 51. Minamida, K., Shiga, K., Sujaya, I. N., Sone, T., Yokota, A., Hara, H., Asano, K., and Tomita, F. (2005) Effects of difructose anhydride III (DFA III) administration on rat intestinal microbiota, Journal of Bioscience and Bioengineering 99, 230-236. 52. Tamura, A., Mita, Y., Shigematsu, N., Hara, H., and Nishimura, N. (2006) Different effects of difructose anhydride III and inulin-type fructans on caecal microbiota in rats, Archives of Animal Nutrition 60, 358-364. 53. Deslongchamps, P. (1975) STEREOELECTRONIC CONTROL IN CLEAVAGE OF TETRAHEDRAL INTERMEDIATES IN HYDROLYSIS OF ESTERS AND AMIDES, Tetrahedron 31, 2463-2490. 54. Koutek, B., Prestwich, G. D., Howlett, A. C., Chin, S. A., Salehani, D., Akhavan, N., and Deutsch, D. G. (1994) INHIBITORS OF ARACHIDONOYL ETHANOLAMIDE HYDROLYSIS, Journal of Biological Chemistry 269, 22937-22940. 55. Clifford, M. N. (1999) Chlorogenic acids and other cinnamates - nature, occurrence and dietary burden, Journal of the Science of Food and Agriculture 79, 362-372. 56. Vanhoof, G., Goossens, F., Demeester, I., Hendriks, D., and Scharpe, S. (1995) PROLINE MOTIFS IN PEPTIDES AND THEIR BIOLOGICAL PROCESSING, Faseb Journal 9, 736-744. 57. Dinh, T. P., Carpenter, D., Leslie, F. M., Freund, T. F., Katona, I., Sensi, S. L., Kathuria, S., and Piomelli, D. (2002) Brain monoglyceride lipase participating in endocannabinoid inactivation, Proceedings of the National Academy of Sciences of the United States of America 99, 10819-10824. 58. Freeman, G. G., and Hopkins, R. H. (1936) The mechanism of degradation of starch by amylases. III. Mutarotation of fission products, Biochemical Journal 30, 451-456. 59. Yang, C. H., Huang, Y. C., Chen, C. Y., and Wen, C. Y. (2010) Expression of Thermobifida fusca thermostable raw starch digesting alpha-amylase in Pichia pastoris and its application in raw sago starch hydrolysis, Journal of Industrial Microbiology & Biotechnology 37, 401-406. 60. Withers, S. G. (2001) Mechanisms of glycosyl transferases and hydrolases, Carbohydrate Polymers 44, 325-337. 61. Zhang, Y. H. P., and Lynd, L. R. (2004) Toward an aggregated understanding of enzymatic hydrolysis of cellulose: Noncomplexed cellulase systems, Biotechnology and Bioengineering 88, 797-824. 62. Irvine, J. C., and Steele, E. S. (1915) The mechanism of mutarotation in aqueous solution, Journal of the Chemical Society 107, 1230-1240. 63. Capon, B., and Walker, R. B. (1974) KINETICS AND MECHANISM OF MUTAROTATION OF ALDOSES, Journal of the Chemical Society-Perkin Transactions 2, 1600-1610. 64. Guderian, A., Dechert, G., Zeyer, K. P., and Schneider, F. W. (1996) Stochastic resonance in chemistry .1. The Belousov-Zhabotinsky reaction, Journal of Physical Chemistry 100, 4437-4441. 65. Cervellati, R., Honer, K., Furrow, S. D., Neddens, C., and Costa, S. (2001) The Briggs-Rauscher reaction as a test to measure the activity of antioxidants, Helvetica Chimica Acta 84, 3533-3547. 66. Kolaranic, L., and Schmitz, G. (1992) MECHANISM OF THE BRAY-LIEBHAFSKY REACTION - EFFECT OF THE OXIDATION OF IODOUS ACID BY HYDROGEN-PEROXIDE, Journal of the Chemical Society-Faraday Transactions 88, 2343-2349. 67. Lambert, J. L., and Fina, G. T. (1984) IODINE CLOCK REACTION-MECHANISMS, Journal of Chemical Education 61, 1037-1038. | |
| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/48223 | - |
| dc.description.abstract | 拉曼光譜學是用來研究分子與晶格的振動及旋轉模式的分析技術. 拉曼散射,一種光的非彈性散射, 是由觀察者C.V.Raman的名字來命名. 自從這位印度科學家在1928年利用太陽光觀察到此現象, 科學家們便逐漸的開始對拉曼散射產生興趣. 有別於其他分析技術, 拉曼光譜學有著以下特點.
第一點, 由於拉曼光譜學是一種光學分析技術, 所以是一種非侵入式且非破壞的分析方法. 第二點, 不同的分子其化學結構與鍵結必定有所不同, 使得他們擁有獨一無二的振動模式. 若利用拉曼光譜學來進行分析, 就可以獲得高專一性的分子指紋. 這項特點讓拉曼光譜學可以輕易的分辨出同分異構物的差異, 這是其他分析方法如質譜儀無法辦到的.第三點, 樣品製備的條件門檻相對簡單. 無論是固態, 液態或氣態, 有機物或無機物都可以進行分析. 樣品本身也不需經過特殊處理, 這是紅外線吸收光譜等分析技術無法相比的. 另外由於只有雷射光源照射到的部分才會產生拉曼散射, 所以樣品的體積可以十分微小 (雷射光點大小約 2 微米). 如果是玻璃或石英包裝樣品, 甚至可以透過包裝直接進行分析而不需拆封. 最後一點, 現在市面上已經有許多商業化的拉曼光譜分析儀器, 使用起來相當簡單, 只需幾秒鐘就可以得到所需的資料. 綜合上述優點, 拉曼光譜分析學已經成為現今相當有力的化學分析方法. 為了進一步改善, 而其他相關的拉曼光譜技術也被後人陸續發展出來. 例如表面增強拉曼光譜學 (可增強拉曼訊號強度), 顯微拉曼光譜學 (可改善空間解析度)以及共振拉曼光譜學 (可取得特殊資訊). 此論文可以概分為兩大研究主軸. 在第一部分中, 我們親自架設了一套探針增強式拉曼光譜系統. 並利用此系統當作分析工具, 藉由其同時擁有表面增強式拉曼光譜的訊號加強以及原子力顯微鏡的高空間解析度的優點, 進一步觀察石墨表面上的奈米尺度缺陷. 同時, 根據實驗的數據結果, 我們也提出一方法來評估此探針增強式拉曼光譜系統在量測如石墨這類非均相物質時的訊號增強係數. 在第二部分, 我們試著利用拉曼光譜技術進一步探討醣類分子在進行水解反應時的反應機制與動力學. 醣水解反應在中性以及弱酸環境被認為是一種由於質子濃度增加以至於溶液酸鹼度降低的自催化反應, 但是卻缺乏直接的證據證明真正的催化物為何. 在此, 我們藉由在不同的反應溫度(80~100℃)與溶液酸鹼度(pH1~pH5)進行兩種雙醣系統(雙果醣以及纖維二醣)的水解反應, 來觀察醣類水解時自催化反應的真正催化物為何, 並且推論出一反應機制來解釋此現象. 這項重大的發現或許可以使得纖維素等多醣體的水解反應效率大幅提升. | zh_TW |
| dc.description.abstract | Raman spectroscopy is a method to observe the vibration behavior of molecules when they are excited by photons. Since C.V. Raman discovered the Raman scattering effect in 1928, people have gradually paid their attention on this interesting subject. Compare with other analytical techniques, Raman spectroscopy has several distinguishing features.
First, this is an optical methodology thus no destructive damage or invasive behavior will take place. Second, each molecule has its own chemical structure so their vibration modes are highly specific like a chemical fingerprint. Isomers can be distinguished easily even they have identical chemical structure formula and molecular weight. Third, the demands for sample preparation are relative simple. It could be organic or inorganic; solids, liquids or gas. And because the laser spot size is only 1~2 | en |
| dc.description.provenance | Made available in DSpace on 2021-06-15T06:49:23Z (GMT). No. of bitstreams: 1 ntu-100-D94223029-1.pdf: 5986605 bytes, checksum: 983b33a05b9ab546d5057a193d774bdc (MD5) Previous issue date: 2011 | en |
| dc.description.tableofcontents | Acknowledgement …………………………………………………………….… I
Chinese layout …………….……………………………………………………… II English layout ………………..……………………………….………………… IV Catalog …………………………………………………………………………... VI Figure content …………………………………………………………………… XI Abbreviation …………….……………………………………………………… XV PART 1 Using Tip-Enhanced Raman Spectroscopy as a Tool for Nano-scale Materials Identification. Abstract …………………………………………………………………………… 2 Chapter 1 Introduction ………………………………………………….………. 3 1.1 Purpose of this work ……………………………………………..………. 3 1.2 Raman spectroscopy ………………………………………….….………. 4 1.2.1 Historical background ……………………………..…….…..….. 4 1.2.2 Basic principles …………………………………………..…..…. 5 1.2.3 Applications ……………………………………………..……… 6 1.3 Atomic force microscopy (AFM) ……………….…………………..…… 9 1.3.1 Contact mode ………………….……....……………………..... 10 1.3.2 Non-contact mode ………….……..….………………….…….. 10 1.3.3 Taping mode ………………...……..….……………..………… 11 1.4 Surface enhanced Raman spectroscopy (SERS) ……………….………. 11 1.4.1 Electromagnetic theory ………………...……………..……….. 13 1.4.2 Chemical theory ……………………...……….……..………… 14 1.5 Tip-enhanced Raman spectroscopy (TERS) ………...…………..……… 15 1.5.1 Principle of TERS ……………………………….…………….. 15 1.6 Allotropes of carbon …………………………...………………..……… 16 1.6.1 Importance of carbon allotropes ………………………………. 16 1.6.2 Types of carbon allotropes …………………..………………… 17 1.6.2.1 Graphite ……………………………………..…………… 17 1.6.2.2 Graphene ……………………………………...……….… 19 1.6.2.3 Fullerene ……………………………………...………….. 21 1.7 Graphite and graphite defects ……………………………………….….. 24 1.7.1 Difference in Raman spectra ……………………….………….. 25 1.7.2 Explanations ………………………………………...…………. 26 1.8 Focused ion beam (FIB) ……………………………………...………… 27 1.8.1 Basic principles ……………………………………..……….… 27 1.8.2 Applications ………………………………………...…………. 29 Chapter 2 Experiments …………………………………………….………….. 31 2.1 Instrument …………………………………………………….………… 31 2.1.1 Focused ion beam (FIB) ……………………………………….. 31 2.1.2 Sputtering chamber ………………………………...………….. 31 2.1.3 Scanning electron microscopy (SEM) ………………………… 32 2.1.4 TERS system …………………………………………..…….… 33 2.2 Sample preparation ……………………………………………...……… 35 2.2.1 SiC nanoislands on Si substrate …………………….…………. 35 2.2.2 FIB bombarded graphite ………………………………………. 36 2.2.3 Ag coated tip ……………………………………….………..… 38 Chapter 3 Results and Discussion …………………………………………….. 42 3.1 Fabrication of Ag coated tips ………………………………..……..…… 42 3.1.1 Quality control of Ag coated tips ……………………………… 42 3.1.2 Optimize protocols for making a “good” tip …….……………. 43 3.1.3 Single Ag bead on tip apex by FIB bombardment ………….… 44 3.2 SERS of graphite defect ………………..………………….…………… 45 3.3 Polarization dependence of graphite defect ……..………..……………. 48 3.3.1 Graphite sample with native well-orientate defects …………… 48 3.3.2 Experimental data ……………………………….…………….. 49 3.4 TERS of graphite defect ……………..……..……………...…………… 51 3.4.1 Native graphite defect …………………………………………. 51 3.4.2 FIB bombarded graphite defect ……………..………………… 52 3.5 Evaluation of enhancing power ……………………..….…………….… 54 Chapter 4 Conclusion …………………………………………………………. 57 4.1 Establishing protocols to fabricate “good” tips for TERS …………..….. 57 4.2 Demonstration of TERS on FIB-irradiated graphite defect …..……..….. 57 4.3 Calculate the enhancing power of anisotropic materials ………….……. 58 Reference ……………………………………………………………………….... 59 PART 2 Monitoring the Hydrolysis of Saccharides with Raman Spectroscopy Abstract ………………………………………………………………………….. 70 Chapter 1 Introduction ………………………………………………………… 71 1.1 Purpose of this work ……………………………………..……………... 71 1.2 Carbohydrates ………………...………………………………..……….. 72 1.2.1 Importance of carbohydrates …………………..…….………… 72 1.2.2 Monosaccharides …………………………..………….……..… 73 1.2.2.1 Glucose ………………………………..………….……… 75 1.2.2.2 Fructose ……………………………………………..…… 77 1.2.3 Disaccharides ………………………...…………….………..… 79 1.2.3.1 Cellobiose …………………………………………..…… 79 1.3 Difructose anhydrides …………………………………………..……… 80 1.4 Hydrolysis of saccharides ………………………..………….……….… 81 1.4.1 Glycosidic bond ………………………………………..……… 81 1.4.2 Mechanism ……………………..……………………………… 82 1.5 Mutarotation ………………………………..……………………..….… 84 1.6 Autocatalytic reaction ………………..……………………………….… 85 1.6.1 Reaction orders ……………………………….……………..… 86 1.6.2 Examples ………………………………………………….…… 87 Chapter 2 Experiment ……………………..…………………………...……… 88 2.1 Sample preparation ……………..…………………...…………..……… 88 2.2 Instrumental setup ………………………………….………….…..…… 89 2.3 Theoretical calculation ……………………………..…….………..…… 89 2.4 Monitoring of DFA III hydrolysis …………………..……………..…… 90 2.4.1 Raman spectra of DFA III powder and solution …………….… 90 2.4.2 DFA III hydrolysis with different temperature (80~100℃) ....… 90 2.4.3 DFA III hydrolysis in strong acid (pH1~pH3) …..………...… 90 2.4.4 DFA III hydrolysis with catalyst (fructose) assistance ….…… 91 2.4.5 DFA III hydrolysis in weak acid with catalyst assistance …… 91 2.5 Hydrolysis of Cellobiose w/o catalyst (glucose) assistance ….…..…… 91 Chapter 3 Results and Discussion ………..….……………………….……… 92 3.1 Difructose anhydride III …………………….………………..…..…… 92 3.1.1 Raman spectrum of DFA III ………………………………….. 92 3.1.2 Peak assignment of DFA III ...………………….….…….…… 93 3.1.3 pH effect on Raman spectra ……………………….….……… 95 3.1.4 DFA III hydrolysis …..……………………………….…….… 95 3.1.5 DFA III hydrolysis with different temperature ………….…… 97 3.1.6 DFA III hydrolysis with catalyst (fructose) assistance …….… 99 3.1.7 DFA III hydrolysis in weak acid with catalyst assistance.…… 100 3.2 Reaction kinetics …………………..……………………….………..… 101 3.3 Mechanism of autocatalytic reaction in DFA III hydrolysis …….…..… 103 3.4 Hydrolysis of cellobiose ………………………………..…….……..… 104 3.4.1 Cellobiose hydrolysis in strong acid…………………….….… 105 3.4.2 Cellobiose hydrolysis with catalyst (glucose) ……………...… 107 Chapter 4 Conclusion ………..………………………………………….…… 109 4.1 Establish a fundamental basis of Raman spectra of DFAs ……..…...… 109 4.2 Observation of new autocatalytic pathway …………………….……… 109 Reference ……………………………………………………………………….. 111 | |
| dc.language.iso | zh-TW | |
| dc.subject | 雙果醣 | zh_TW |
| dc.subject | 拉曼 | zh_TW |
| dc.subject | 探針增強式拉曼 | zh_TW |
| dc.subject | 石墨 | zh_TW |
| dc.subject | 醣 | zh_TW |
| dc.subject | 水解 | zh_TW |
| dc.subject | 自催化反應 | zh_TW |
| dc.subject | Raman spectroscopy | en |
| dc.subject | autocatalytic reaction | en |
| dc.subject | difructose anhydride (DFA) | en |
| dc.subject | hydrolysis | en |
| dc.subject | glycosidic bond | en |
| dc.subject | disaccharides | en |
| dc.subject | graphite | en |
| dc.subject | tip-enhanced Raman spectroscopy (TERS) | en |
| dc.title | 藉由拉曼光譜偵測奈米尺度物質以及研究化學反應動力學 | zh_TW |
| dc.title | Using Raman Spectroscopy for Nanoscale Material Detection and Chemical Reaction Kinetics Study | en |
| dc.type | Thesis | |
| dc.date.schoolyear | 99-2 | |
| dc.description.degree | 博士 | |
| dc.contributor.coadvisor | 王玉麟(Yuh-Lin Wang) | |
| dc.contributor.oralexamcommittee | 王俊凱(Jun-Kai Wang),林景泉,劉志毅 | |
| dc.subject.keyword | 拉曼,探針增強式拉曼,石墨,醣,水解,自催化反應,雙果醣, | zh_TW |
| dc.subject.keyword | Raman spectroscopy,tip-enhanced Raman spectroscopy (TERS),graphite,disaccharides,glycosidic bond,hydrolysis,difructose anhydride (DFA),autocatalytic reaction, | en |
| dc.relation.page | 119 | |
| dc.rights.note | 有償授權 | |
| dc.date.accepted | 2011-03-17 | |
| dc.contributor.author-college | 理學院 | zh_TW |
| dc.contributor.author-dept | 化學研究所 | zh_TW |
| 顯示於系所單位： | 化學系 | |
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