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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 張煥宗(Huan-Tsung Chang) | |
dc.contributor.author | Kun-Hong Li | en |
dc.contributor.author | 李昆鴻 | zh_TW |
dc.date.accessioned | 2021-06-14T17:00:36Z | - |
dc.date.available | 2008-08-05 | |
dc.date.copyright | 2008-08-05 | |
dc.date.issued | 2008 | |
dc.date.submitted | 2008-07-28 | |
dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/40794 | - |
dc.description.abstract | 隨著奈米科技的進步,許多相關性的研究也隨之日新月異與蓬勃發展。本論文之研究目的在於製備不同的金銀奈米材料與二氧化鈦奈米粒子(titanium dioxide nanoparticles, TiO2 NPs),並將其應用於分析胺基硫醇分子(aminothiols)與多酚類化合物(polyphenolic compounds)。另一方面,我們也嘗試利用毛細管電泳搭配雷射誘導螢光(CE-LIF)的技術來探討不同序列之DNA分子與汞離子之間的作用。論文的第一部份簡述了奈米材料的製備、物理及化學性質同時也介紹了與本論文相關之實驗技術。在第二部份的研究中我們利用尼羅紅(Nile red)修飾的金奈米粒子(NR-Au NPs)來瞭解硫醇分子與金奈米粒子之間的相互作用。藉由觀察硫醇分子加入NR-Au NPs溶液中所產生的螢光變化,不同硫醇分子的吸附速率可以利用Langmuir isotherm model來推算得知。而從實驗結果可以得知硫醇分子的吸附速率與本身的立體結構與電荷有關,同時也取決於奈米粒子的粒徑大小。此外,對於NR吸附在金奈米粒子的表面上進而形成NR產物的催化反應也在本章節中被詳細的探討。第三部份的研究主要是利用晶種促進成長法(seed-mediated growth method)在玻璃基材上製備各種金和銀奈米材料。藉由調控金和銀的晶種濃度我們可在基材上製備出高產率(27% 和54%)、高均勻性以及大尺寸(1.36 和5.21 μm)的金和銀奈米材料。藉由暗場顯微鏡(dark-field microscopy, DFM)與掃瞄式電子顯微鏡(scanning electron microscopy, SEM)的量測,這些在基材上已製備好的奈米材料可以被快速的觀察與鑑定。除此之外,從單一金屬的散射光譜圖也可以清楚地瞭解每一種奈米材料之表面特性。最後,將此製成方法與DFM的分析技術做一結合,則可以成功地在基材表面上進行高通量(high-throughput)的製備與鑑定金奈米材料的大小與形狀。第四部份的研究則是選擇TiO2 NPs作為表面輔助雷射脫附游離質譜法(surface-assisted laser desorption/ionization mass spectrometry, SALDI-MS)的基質並具備探針性質可以選擇性的偵測兒茶素分子(catechins)。透過TiO2 NPs對烯二醇類(enediol)官能基化合物之高親和作用力與藉由能量轉移所增強吸收紫外光之特性,TiO2 NPs 可有效地當作SALDI-MS的輔助基質來對兒茶素分子進行選擇性的分析。此分析方法已被證實可以成功地應用於分析與定量茶類中之兒茶素、維他命C與茶胺酸分子,亦即表示此技術未來應用於生命科學之極大潛力。最後一部份的研究則是利用CE-LIF的技術來探討DNA分子在汞離子的作用下其分離的結果並試著開發一簡單及快速分離小片段單股DNA的方法。其原理主要為透過汞離子與胸腺嘧啶(thymine, T)鹼基之間所形成的的特殊鍵結T-Hg2+-T來調控這些DNA分子的構形,再利用毛細管中填充之中性的聚合物溶液(聚環氧乙烷,簡稱PEO)來篩分這些DNA分子。隨著改變分離溶液中汞離子的濃度,4條DNA分子T33, C5T28, T5C5T23和 T15C5T13可在20分鐘內被逐漸的解析開來,且其分離時間之相對標準偏差小於2.5%。此4條DNA分子在分離過程中所產生的電淌 (mobility)差異除了與汞離子所誘導的構形不同有關,同時DNA分子與汞離子作用之後所產生的電荷密度差異也會影響其分離的結果,而此推論隨後也藉由螢光及圓二光偏極光譜(circular dichroism)的量測來得到證實。 | zh_TW |
dc.description.abstract | With the growing advances in nanotechnology, a number of interesting related researches have been demonstrated. In this thesis, we mainly focus on the preparation of different kinds of nanomaterials including gold, silver, titanium dioxide, and on their applications to the analysis of aminothiols and polyphenolic compounds. In addition, capillary electrophoresis (CE) in conjunction with laser-induced fluorescence (LIF) has been conducted to study the interactions of DNA with Hg2+. We briefly describe preparation, physical and chemical properties of nanomaterials as well as introduce related techniques used in this thesis in Chapter 1. In Chapter 2, the interactions between a variety of thiols and Nile Red-adsorbed gold nanoparticles (NR-Au NPs) by monitoring the fluorescence changes of NR-Au NPs solutions are described. Using the Langmuir isotherm model, the displacement rate constants of the NR product from the Au NP surface are estimated. Our results reveal that steric effects and the charge density of the thiols both play important roles in determining the interactions with NR-Au NPs. The interactions are also dependent on the size of NR-Au NPs. Furthermore, the catalytic characteristics of Au NPs have also been proposed through the formation of an NR product from NR upon the Au NP surface. In Chapter 3, we demonstrate the preparation of Au and Ag nanomaterials from their corresponding colloidal seeds on glass substrates via a seed-mediated growth method. By carefully controlling the concentrations of Au and Ag nanoparticle seeds, different sizes and shapes of Au and Ag nanomaterials with narrow size distribution, higher yields (27% and 54%), and larger sizes (1.36 and 5.21 μm) can be prepared. Through dark-field microscopy (DFM) and SEM measurements, the thus-prepared nanomaterials were easily and rapidly characterized. From the scattering spectra of single Au and Ag nanomaterials, we obtaibned more detailed information about their morphologies. Combining our synthetic method with DFM system, the high-throughput preparation and characterization of differently sized and shaped Au nanomaterilas on a glass substrate can be achieved. We discuss use of titanium dioxide nanoparticles (TiO2 NPs) as selective probes and matrices for the determination of catechins through surface-assisted laser desorption/ionization mass spectrometry (SALDI-MS) in Chapter 4. Due to the high specificity of TiO2 NPs towards enediol-containing compounds as well as their strong absorption characteristics through efficient energy transfer, TiO2 NPs serve as affinity probes and as effective LDI matrices for the SALDI-MS determination of catechins. This method has been validated in the analysis of catechins, ascorbic acid and theanine in tea samples, showing its great potential for applications in life sciences. In Chapter 5, we discuss a simple and fast CE-LIF method for separation of short ssDNA fragments in the presence of Hg2+. Through the specific interaction of Hg2+ ions with thymine-thymine (T-T) base pairs of the DNAs, four ssDNA, including T33, C5T28, T5C5T23, and T15C5T13 were successfully separated by CE using poly(ethyleneoxide) (PEO) solutions. The separation of the four DNA fragments were completed within 20 min, with the relative standard deviation values all less than 2.5%. The Hg(II)-induced changes in conformation and charge density in the DNA are responsible for their changes in mobility during separation. Our reasoning is further supported by the fluorescence and ellipticity spectra. | en |
dc.description.provenance | Made available in DSpace on 2021-06-14T17:00:36Z (GMT). No. of bitstreams: 1 ntu-97-F92223006-1.pdf: 2654189 bytes, checksum: f97cafc64cbf2cb670157c8c6e310591 (MD5) Previous issue date: 2008 | en |
dc.description.tableofcontents | 中文摘要 I
Abstract III Contents V Table contents IX Figure contents IX Conclusions and Prospects 139 1. Introduction 1 1.1 Nanomaterials 2 1.1.1 Optical Properties 3 1.1.2 Classification of Nanomaterials 4 1.1.2.1 Gold Nanoparticles (Au NPs) 4 1.1.2.2 Gold Nanorods (Au NRs) 5 1.1.2.3 Titanium Dioxide (TiO2) NPs 7 1.2 Applications 8 1.2.1 Imaging 8 1.2.2 Catalysis 10 1.2.3 Sensing 11 1.2.3.1 Absorption-Based Method 11 1.2.3.2 Scattering-Based Detection 13 1.2.3.3 Fluorescence-Based Detection 14 1.2.4 Nanomaterials for Laser Desorption/Ionization Mass Spectrometry 15 1.3 Capillary Electrophoresis for DNA Analysis 17 1.3.1 Capillary Electrophoresis 17 1.3.2 Importance and Modes of Metal Ion Binding to Nucleic Acids 19 1.3.3 Electrophoretic Approaches for DNA Analysis 21 1.3.4 Separation Mechanisms 22 1.4 Motive of Research 24 1.5 References 25 2. Fluorescence and Interactions With Thiol Compounds of Nile Red-Adsorbed Gold Nanoparticles 38 2.1 Introduction 39 2.2 Experimental Section 40 2.2.1 Chemicals 40 2.2.2 Synthesis of 14-, 32, and 56-nm-Diameter Au NPs 41 2.2.3 Preparation of NR-Au NPs 41 2.2.4 Characterization of Au NPs and NR-Au NPs 42 2.2.5 Measurements of the Molecular Mass of the NR Product 43 2.2.6 Coverage of NR on Au NPs 43 2.2.7 Kinetic Measurements of NR Adsorption 43 2.2.8 Kinetic Measurements of the Displacement Rate of the NR Products by Thiols 44 2.2.9 Analysis of Kinetic Data 44 2.2.10 FT-IR Measurement 44 2.3 Results and Discussion 45 2.3.1 Formation of the NR Product 45 2.3.2 Kinetic Measurements of NR Adsorption and Rates of Thiol Displacement 46 2.3.3 Effect of Au NP Size 51 2.4 Conclusions 51 2.5 References 52 3. Manipulation of the Growth of Gold and Silver Nanomaterials on Glass by Seeding Approach 64 3.1 Introduction 65 3.2 Experimental Section 67 3.2.1 Chemicals 67 3.2.2 Functionalization of Glass Substrates 67 3.2.3 Growth of Au Nanomaterials on Glass Slides 68 3.2.4 Growth of Ag Nanomaterials on Glass Slides 68 3.2.5 Multiplexed Synthesis System 69 3.2.6 Instrumentation 69 3.3 Results and Discussion 70 3.3.1 Effect of Seed Concentration on the Growth of Au and Ag Nanomaterials 70 3.3.2 Growth Kinetics of Au and Ag Nanomaterials 74 3.3.3 DFM Images and UV-Vis Spectra for Single Ag and Au Nanomaterials 76 3.3.4 Multiplexed Synthesis of Au Nanomaterials 78 3.4 Conclusions 79 3.5 References 79 4. Determining Enediol Compounds in Tea Using Surface-Assisted Laser Desorption/Ionization Mass Spectrometry With Titanium Dioxide Nanoaprticle Matrices 97 4.1 Introduction 98 4.2 Experimental Section 100 4.2.1 Chemicals 100 4.2.2 Preparation of TiO2 NPs 101 4.2.3 Characterization of TiO2 NPs 101 4.2.4 Determination of Catechins 101 4.2.5 Preparation of Standard Solutions 102 4.2.6 Analysis of Tea Samples 102 4.2.7 MALDI-TOF and SALDI-TOF MS Measurements 103 4.3 Results and Discussion 103 4.3.1 Optical Properties of TiO2 NPs 103 4.3.2 TiO2 NPs as Assisted Matrices in SALDI-MS 104 4.3.3 Quantitative Analyses of Three Model Catechins 107 4.3.4 Determination of EGC and EGCG in Tea Samples 107 4.4 Conclusions 108 4.5 References 108 5. Screening Aptamers for Mercury (II) by Capillary Electrophoresis 120 5.1 Introduction 121 5.2 Materials and Methods 124 5.2.1 Chemicals and Capillary 124 5.2.2 Apparatus 124 5.2.3 Preparation of Polymer Solutions Containing Hg2+ ions 125 5.2.4 DNA Separation by CE 125 5.2.5 Fluorescence and CD Measurements 126 5.3 Results and Discussion 126 5.3.1 Effect of the Concentrations of Hg2+ on the DNA Separation 126 5.3.2 Fluorescence and CD Measurements 128 5.4 Conclusions 129 5.5 References 130 | |
dc.language.iso | zh-TW | |
dc.title | 金與二氧化鈦奈米粒子之合成、表面修飾及其應用 | zh_TW |
dc.title | Synthesis, Surface Modification, and Applications of
Nanomaterials: Gold and Titanium Dioxide | en |
dc.type | Thesis | |
dc.date.schoolyear | 96-2 | |
dc.description.degree | 博士 | |
dc.contributor.oralexamcommittee | 劉春櫻(Chuen-Ying Liu),陳俊顯(Chun-hsien Chen),周禮君(Lai-Kwan Chau),柯富祥(Fu-Hsiang Ko) | |
dc.subject.keyword | 金奈米粒子,二氧化鈦奈米粒子, | zh_TW |
dc.subject.keyword | gold nanoparticles,titanium dioxide nanoparticles, | en |
dc.relation.page | 137 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2008-07-30 | |
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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