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http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/67990完整後設資料紀錄
| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 鄭如忠(Ru-Jong Jeng) | |
| dc.contributor.author | Chia-Yen Chiang | en |
| dc.contributor.author | 江佳晏 | zh_TW |
| dc.date.accessioned | 2021-06-17T02:02:33Z | - |
| dc.date.available | 2027-07-17 | |
| dc.date.copyright | 2017-07-20 | |
| dc.date.issued | 2017 | |
| dc.date.submitted | 2017-07-18 | |
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/67990 | - |
| dc.description.abstract | 本實驗成功開發一新型的表面增強拉曼散射基板(surface-enhanced Raman scattering substrates, SERS substrates)，因具有三維規則蜂窩狀孔洞結構，將可有效地改善拉曼訊號之偵測靈敏度及再現性，應用於快速檢測多種化合物。
此三維規則排列之蜂窩狀孔洞結構以polyurethane-co-azetidine-2,4-dione (PU-PAZ)作為材料，於呼吸法(breath figure method)的製備方式中，PU-PAZ高分子結構中的兩性型樹枝狀高分子能穩定水分子及高分子溶液間的界面，並控制水分子整齊排列於溶液表面或深入其中的自組裝現象，等到水分子及溶劑完全揮發即得到規整的孔洞結構。以不同相對濕度及高分子溶液濃度來調控孔洞大小及排列整齊度，再附著金奈米粒子製備出多層孔洞結構之SERS基板，與表面具金之平膜基板比較SERS放大效果。 基板的檢測靈敏度將以增強因子(enhancement factors, EF)來量化，計算具有孔洞結構SERS基板的EF值約為106，遠大於對照組的平膜SERS基板(平膜基板之EF值為104)。接著以不同深度的共軛焦拉曼光譜掃描及SEM圖像，佐證本實驗所推論於兩種結構的SERS放大機制差異，顯示多孔洞SERS基板因表面及三維孔洞結構中皆佈滿金奈米粒子，可由鄰近粒子間的熱點效應(hot-spots resonance effects)，大幅增強散射於金屬表面電磁場之待測物拉曼訊號；此外，雷射可於孔洞腔體進行多次反射，可增加被照射之金奈米粒子因表面電漿子共振(surface plasmon)產生熱點效應的機率，因此，三維孔洞基板同時有表面及孔洞內部加成的SERS訊號，故較二維平面之基板擁有較優良之SERS效應。 本實驗亦討論金奈米粒子的粒徑大小、孔洞結構之表面形貌等變因，對SERS基板檢測能力的影響，結果顯示粒徑較大之金奈米粒子可引發較強之熱點效應，能增進基板偵測靈敏度；而孔洞大小及排列規則度也對訊號偵測靈敏度及再現性扮演重要的因素。該SERS基板除了能快速放大極微量待測物的拉曼訊號以利檢測，亦可用於不同化合物分子的偵測，如在針對R6G分子的偵測極限濃度(Limitation of detection, LOD)可達到10-8 M，且找到濃度介於10-5至10-8 M的檢量線以利未來的應用。 關鍵字：表面增強拉曼散射、蜂窩狀孔洞結構、呼吸法、金奈米粒子、熱點效應 | zh_TW |
| dc.description.abstract | Novel surface-enhanced Raman scattering (SERS) substrates with three-dimensional (3D) porous structures have been developed for effectively improving the sensitivity and reproducibility of SERS, which can rapidly detect small molecules. Periodical arrays of the honeycomb-like substrates were fabricated by self-assembling polyurethane-co-azetidine-2,4-dione (PU-PAZ) polymers. PU-PAZ comprising amphiphilic dendrons could stabilize the interfaces between the water droplets and polymer solution, and then organize into regular porous structures through the breath figure method. Subsequently, SERS substrates were fabricated by immobilizing gold nanoparticles (AuNPs) onto the polymer films with various 3D honeycomb-like porous structures, controlled by different PU-PAZ concentrations and relative humidities. Results show that surface enhancement factors of honeycomb-like substrates as large as 106 are much higher than that of flat-film substrates (control group) due to enormous accumulation of hot-spots resonance effects in the 3D porous structure as verified through Raman mapping at various positions of the z-axis. Furthermore, the particle size effects were evaluated by immobilized different sizes of AuNPs on the honeycomb-like substrates, indicating larger AuNPs could induce more pronounced hot-spots effects as verified by the broad scattering peak of aggregating AuNPs. The generation of hot-spots resonance to enhance Raman intensity is strongly dependent on the diameter of AuNPs, the pore sizes and distributions of the 3D honeycomb-like porous substrates. Such substrates are ready for label-free and rapid SERS detection.
Keywords：surface-enhanced Raman scattering (SERS); breath figure; honeycomb-like polymeric films; gold nanoparticles; hot-spots resonance effects. | en |
| dc.description.provenance | Made available in DSpace on 2021-06-17T02:02:33Z (GMT). No. of bitstreams: 1 ntu-106-R04549007-1.pdf: 8883155 bytes, checksum: d13ea88e07e510857247c72559bfdb5c (MD5) Previous issue date: 2017 | en |
| 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 3 2.1 具表面微結構之蜂窩狀高分子材料 3 2.1.1 Breath Figures法之機制 3 2.1.2 應用於Breath Figures方法之高分子 6 2.1.2.1 規則樹枝狀高分子應用於製備蜂窩狀孔洞高分子膜 11 2.1.2.2 poly(urea/malonamide) dendrons應用於製備蜂窩狀孔洞高分子膜 16 2.2 表面增強拉曼散射 24 2.2.1 拉曼光譜之簡介及原理 24 2.2.2 表面增強拉曼散射之簡介及原理 25 2.2.3 表面增強拉曼散射之應用 27 2.3 金奈米粒子 28 2.3.1 金奈米粒子之性質與結構 28 2.3.2 金奈米粒子之合成方式及生成機制 31 2.4 研究動機 33 參、實驗內容 34 3.1 藥品及溶劑 34 3.2 實驗儀器 36 3.3 實驗流程圖 38 3.4 實驗步驟 39 3.4.1 金奈米粒子之合成 39 3.4.2 Isocyanato-4’(3,3-dimethyl-2,4-dioxo-azetidino) diphenylmethane (IDD) 之合成 40 3.4.3 C18系列polyurea/malonamide dendrons 之合成 41 3.4.3.1 [G-0.5]-C18之合成 41 3.4.3.2 [G-1]-C18之合成 42 3.4.3.3 [G-1.5]-C18之合成 42 3.4.4 鏈延長劑之合成 42 3.4.4.1 DEA-diol之合成 42 3.4.4.2 [G-1.5]-C18-diol之合成 43 3.4.5 側鏈具反應官能基之PU-PAZ高分子之合成 44 3.4.6 規則蜂窩狀孔洞高分子薄膜之製備 44 3.4.7 平滑高分子薄膜之製備 45 3.4.8 具金奈米粒子之蜂窩狀孔洞SERS基板之製備 45 3.4.9 表面具金奈米粒子之平膜SERS基板之製備 45 3.4.10 表面增強拉曼散射之檢測方式 46 肆、結果與討論 47 4.1 金奈米粒子之合成及鑑定 47 4.2 IDD之合成及結構鑑定 50 4.3 C18系列polyurethane/malonamide dendrons 之合成及結構鑑定 53 4.3.1 [G-0.5]-C18之合成及結構鑑定 53 4.3.2 [G-1]-C18之合成及結構鑑定 54 4.3.3 [G-1.5]-C18之合成及結構鑑定 56 4.4 鏈延長劑之合成及結構鑑定 58 4.4.1 DEA-diol之合成及結構鑑定 58 4.4.2 [G-1.5]-C18-diol之合成及結構鑑定 59 4.5 側鏈具反應官能基之PU-PAZ高分子之化學結構分析 61 4.6 不同變因對於規則蜂窩狀孔洞排列之影響 62 4.6.1 高分子溶液濃度對於蜂窩狀孔洞排列之影響 62 4.6.2 相對溼度對於蜂窩狀孔洞排列之影響 64 4.7 具金奈米粒子之蜂窩狀高分子SERS複合基板之分析 65 4.7.1 三維結構對SERS效應之影響及其機制 65 4.7.2 孔徑大小及排列規整度對SERS效應靈敏度及再現性之影響 70 4.7.3 不同金奈米粒子大小對於SERS效應的之影響 74 4.7.4 SERS基板之極限偵測濃度分析 77 4.7.5 SERS基板之應用分析 79 伍、結論及未來展望 81 陸、參考文獻 84 | |
| dc.language.iso | zh-TW | |
| dc.subject | 呼吸法 | zh_TW |
| dc.subject | 金奈米粒子 | zh_TW |
| dc.subject | 蜂窩狀孔洞結構 | zh_TW |
| dc.subject | 表面增強拉曼散射 | zh_TW |
| dc.subject | 熱點效應 | zh_TW |
| dc.subject | surface-enhanced Raman scattering (SERS) | en |
| dc.subject | breath figure | en |
| dc.subject | hot-spots resonance effects | en |
| dc.subject | gold nanoparticles | en |
| dc.subject | honeycomb-like polymeric films | en |
| dc.title | 具金奈米粒子之蜂窩狀孔洞高分子薄膜基板應用於表面增強拉曼散射檢測 | zh_TW |
| dc.title | Gold Nanoparticles Immobilized on Honeycomb-like Polymeric Films for Surface-Enhanced Raman Scattering (SERS) Detections | en |
| dc.type | Thesis | |
| dc.date.schoolyear | 105-2 | |
| dc.description.degree | 碩士 | |
| dc.contributor.coadvisor | 劉定宇(Ting-Yu Liu) | |
| dc.contributor.oralexamcommittee | 童世煌(Shih-Huang Tung),駱俊良(Chun-Liang Lo) | |
| dc.subject.keyword | 表面增強拉曼散射,蜂窩狀孔洞結構,呼吸法,金奈米粒子,熱點效應, | zh_TW |
| dc.subject.keyword | surface-enhanced Raman scattering (SERS),breath figure,honeycomb-like polymeric films,gold nanoparticles,hot-spots resonance effects, | en |
| dc.relation.page | 89 | |
| dc.identifier.doi | 10.6342/NTU201701569 | |
| dc.rights.note | 有償授權 | |
| dc.date.accepted | 2017-07-18 | |
| dc.contributor.author-college | 工學院 | zh_TW |
| dc.contributor.author-dept | 高分子科學與工程學研究所 | zh_TW |
| 顯示於系所單位： | 高分子科學與工程學研究所 | |
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