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| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 鄭如忠 | zh_TW |
| dc.contributor.advisor | Ru-Jong Jeng | en |
| dc.contributor.author | 陳敏顥 | zh_TW |
| dc.contributor.author | Min-Hao Chen | en |
| dc.date.accessioned | 2023-03-19T21:16:41Z | - |
| dc.date.available | 2023-12-26 | - |
| dc.date.copyright | 2022-08-10 | - |
| dc.date.issued | 2022 | - |
| dc.date.submitted | 2002-01-01 | - |
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/83752 | - |
| dc.description.abstract | 本研究成功開發出以多醚-矽烷官能化樹枝狀高分子為基底之表面增強拉曼散射(SERS)基板，因獨特設計之樹枝狀高分子結構具有矽氧烷官能基，可以藉由水解縮合反應與玻璃基板結合，並以多醚基作為還原點原位還原形成銀奈米粒子，利用不同代數之樹枝狀高分子調控奈米銀粒子之分布，期望提升SERS訊號的強度及穩定性。樹枝狀高分子設計以具反應選擇性之雙官能基單體4-isocyanato-4-(3,3-dimethyl-2,4-dioxo-azetidino)-diphenylmethane (IDD)為構築單元，與具多醚基之triethylene glycol monoether (TEGEE)反應，得到末端為多醚基之0.5代樹枝狀分子與diethylenetriamine反應，透過收斂法合成末端多醚基結構且不同代數之poly(urethane/malonamide)規則樹枝狀高分子，再以3-氨基丙基三乙氧基矽烷(APTES)進行化學改質，合成具矽烷官能基之樹枝狀高分子，且成功透過溶膠凝膠法與氫氧基化玻璃基板進行表面化學反應，將樹枝狀高分子修飾在玻璃表面，形成矽烷化基板；由樹枝狀高分子之羰基與末端醚基作為銀奈米粒子之成核點，以原位還原法將奈米銀粒子沉積在基板上，成功製備出矽烷化SERS基板。由於銀奈米粒子於基板之表面型態會影響SERS檢測效果，以不同代數之樹枝狀高分子（0.5-2.5代）及銀離子濃度（0.5-16 mg/mL），可以調控銀奈米粒子於矽烷化基板上的分佈及含量。結果顯示，1.5代樹枝狀高分子之複合材料為奈米銀粒子最佳分散劑，當銀離子達4 mg/mL時，能夠穩定分散還原之銀奈米粒子，且此基板能夠被穩定地應用於偵測腺嘌呤(adenine)生物分子，其偵測極限濃度(LOD)可達到10-8M，濃度介於10-5M至10-8M呈線性關係，且在重複30次測量下，其強度皆落於相對標準差以內。此新穎設計之利用樹枝狀高分子來控制銀奈米粒子尺寸及分佈之SERS基板，具有優異的靈敏度及穩定性，也將有非常大的潛力應用於分散其他種類之金屬奈米粒子，作為新一代無需標定(label-free)生醫及環境檢測晶片之應用。 | zh_TW |
| dc.description.abstract | In this study, nanocomposite thin films based on functionalized dendrons (alkoxysilane-containing dendrons with peripheral ether linkages) with in-situ reduction of silver nanoparticle (AgNPs) have been successfully fabricated for the sensing chips in surface-enhanced Raman scattering (SERS) detection. To develop highly reproducible and ultrasensitive SERS signals, it’s crucial to optimize the density and dispersion of silver nanoparticles on the substrates. Thus, we design the different generations of poly(urea/malonamide) dendrons (0.5, 1.5, and 2.5 generations) with peripheral ether linkages through iterative addition reactions to modulate the distribution of silver nanoparticles. The dendrons with azetidine-2,4-dione group could undergo ring-opening reaction with terminal primary amine of aminopropyltriethoxysilane (APTES). In addition, APTES was one of the most used surface modifiers because its three hydrolysable ethoxy groups could react with the silanol groups from the oxidized glass substrates. Subsequently, SERS substrates were fabricated by the immobilization of the AgNPs on the functionalized dendron-modified substrates by in-situ reduction of AgNO3 in alcohol solution. The anchoring of AgNPs on the substrates was carried out by electrostatic interaction with carbonyl groups and terminal ether linkages of dendrons. We explore the influence of dendrons of different generations, and concentrations of silver ions on SERS effects through SEM images and Raman spectra. The results show that the optimal SERS spectra were found at the 1.5 generation-dendrons with 4mg/mL AgNO3 immobilized on the silanized substrates, exhibiting the more stable, pronounced and linear-quantitative Raman enhancement for detection of adenine (10-5-10-8M), due to the presence of the moderate size and interparticle gap of AgNPs. The limit of detection (LOD) for adenine is lower than 10-8M. Such substrates with excellent sensitivity and stability exhibited high potential for the rapid and label-free SERS detection. | en |
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| dc.description.tableofcontents | 誌謝 i 中文摘要 ii Abstract iii 目錄 iv 圖目錄 vii 表目錄 xi 壹、緒論 1 貳、文獻回顧 2 2.1 生醫檢測之發展 2 2.2 表面增強拉曼散射 2 2.2.1 拉曼光譜之簡介與原理 2 2.2.2 表面增強拉曼散射之簡介與原理 4 2.2.3 表面增強拉曼散射之應用 5 2.2.4 金屬奈米粒子光學性質與應用 6 2.3 有機-無機奈米複合材料 8 2.3.1 製備方式 9 2.3.2 優缺點及應用 12 2.3.3 矽氧烷於表面化學改質之應用 13 2.4 規則樹枝狀高分子 15 2.4.1樹枝狀高分子之簡介 17 2.4.2 Dendrimer合成路徑 18 2.4.3 反應選擇性單體IDD製備規則樹枝狀高分子 19 2.4.4 poly(urea/malonamide) dendrons於SERS之應用 22 2.5 研究動機 24 參、實驗內容 25 3.1 藥品及溶劑 25 3.2 實驗儀器 27 3.3 實驗流程圖 29 3.4 實驗步驟 31 3.4.1 Isocyanate-4’(3,3-dimethyl-2,4-dioxo-azetidino) diphenylmethane (IDD)之合成 31 3.4.2 醚基系列poly(urea/malonamide) dendrons之合成 32 3.4.3 含矽氧烷之poly(urea/malonamide) dendrons合成 36 3.4.4矽烷化樹枝狀高分子薄膜之製備 38 3.4.5具銀奈米粒子之矽烷化SERS平膜基板之製備 39 3.4.6表面增強拉曼散射之檢測方式 40 肆、結果與討論 41 4.1 IDD之合成與結構鑑定 41 4.2 醚基系列poly(urea/malonamide) dendrons之合成及結構鑑定 44 4.2.1 G0.5-TEGEE之合成及結構鑑定 44 4.2.2 G1.0-TEGEE之合成及結構鑑定 45 4.2.3 G1.5-TEGEE之合成及結構鑑定 47 4.2.4 G2.0-TEGEE之合成及結構鑑定 49 4.2.5 G2.5-TEGEE之合成及結構鑑定 51 4.3含矽氧烷之poly(urea/malonamide) dendrons合成及結構鑑定 54 4.3.1 A-G0.5-TEGEE之合成及結構鑑定 54 4.3.2 A-G1.5-TEGEE之合成及結構鑑定 56 4.3.3 A-G2.5-TEGEE之合成及結構鑑定 57 4.4矽烷化高分子薄膜之表面結構鑑定 59 4.4.1 A-G0.5-TEGEE 59 4.4.2 A-G1.5-TEGEE 63 4.4.3 A-G2.5-TEGEE 65 4.5具銀奈米粒子之高分子薄膜之合成與鑑定 67 4.5.1 銀奈米粒子於A-G0.5-TEGEE薄膜基板 67 4.5.2 銀奈米粒子於A-G1.5-TEGEE薄膜基板 69 4.5.3 銀奈米粒子於A-G2.5-TEGEE薄膜基板 71 4.6 具銀奈米粒子之高分子薄膜於SERS檢測之應用 74 4.6.1 不同銀離子濃度對於SERS效應之影響 74 4.6.2 不同代數樹枝狀高分子對SERS效應之影響 78 4.6.3 銀奈米粒子@醚基樹枝狀高分子薄膜基板與不同基板之比較 80 4.6.4 SERS基板之偵測極限濃度分析 82 4.6.5 SERS基板穩定性測試 83 伍、結論 84 陸、參考文獻 85 | - |
| dc.language.iso | zh_TW | - |
| dc.subject | 銀奈米粒子 | zh_TW |
| dc.subject | 溶膠凝膠法 | zh_TW |
| dc.subject | 矽烷化反應 | zh_TW |
| dc.subject | 樹枝狀高分子 | zh_TW |
| dc.subject | 銀奈米粒子 | zh_TW |
| dc.subject | 表面增強拉曼散測檢測 | zh_TW |
| dc.subject | 溶膠凝膠法 | zh_TW |
| dc.subject | 矽烷化反應 | zh_TW |
| dc.subject | 樹枝狀高分子 | zh_TW |
| dc.subject | 表面增強拉曼散測檢測 | zh_TW |
| dc.subject | silver nanoparticles | en |
| dc.subject | silanization | en |
| dc.subject | sol-gel reaction | en |
| dc.subject | surface-enhanced Raman scattering (SERS) | en |
| dc.subject | surface-enhanced Raman scattering (SERS) | en |
| dc.subject | dendrons | en |
| dc.subject | sol-gel reaction | en |
| dc.subject | silanization | en |
| dc.subject | dendrons | en |
| dc.subject | silver nanoparticles | en |
| dc.title | 多醚-矽烷官能化樹枝狀高分子-銀奈米粒子複合基板於SERS檢測之應用 | zh_TW |
| dc.title | Immobilization of silver nanoparticles based on alkoxysilane-containing dendrons with peripheral ether linkages for SERS detection | en |
| dc.type | Thesis | - |
| dc.date.schoolyear | 110-2 | - |
| dc.description.degree | 碩士 | - |
| dc.contributor.coadvisor | 劉定宇 | zh_TW |
| dc.contributor.coadvisor | Ting-Yu Liu | en |
| dc.contributor.oralexamcommittee | 鄭有為;吳建欣 | zh_TW |
| dc.contributor.oralexamcommittee | Yu-Wei Cheng;Chien-Hsin Wu | en |
| dc.subject.keyword | 表面增強拉曼散測檢測,銀奈米粒子,樹枝狀高分子,矽烷化反應,溶膠凝膠法, | zh_TW |
| dc.subject.keyword | surface-enhanced Raman scattering (SERS),silver nanoparticles,dendrons,silanization,sol-gel reaction, | en |
| dc.relation.page | 91 | - |
| dc.identifier.doi | 10.6342/NTU202202135 | - |
| dc.rights.note | 未授權 | - |
| dc.date.accepted | 2022-08-08 | - |
| dc.contributor.author-college | 工學院 | - |
| dc.contributor.author-dept | 高分子科學與工程學研究所 | - |
| 顯示於系所單位： | 高分子科學與工程學研究所 | |
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