快速識別疾病標誌物，對於疾病診斷、癒後和治療監測至關重要，表面增強拉曼散射是一種靈敏檢測光譜分析技術，具有識別分析物的能力，由於其靈敏度足以檢測極低濃度的分子和迅速的分析能力，廣泛應用各個感測技術領域。於目前研究中，開發一種具有快速識別及高穩定性的SERS基材仍然是一個艱難的挑戰。在本實驗中，將使用表面電漿子奈米結構修飾經過高溫熱處理沸石咪唑酯有機框架。多孔的棒狀金銀奈米核殼結構，是由於棒狀金銀奈米核殼結構經由化學電置換，使紅外線可見光波長調整至所使用的拉曼光譜的氦氖波長 (632.8 nm)，放大並顯著增強拉曼探針分子的檢測訊號。
最後，因為表面電漿子奈米結構所修飾的ZIF-8衍生之奈米多孔碳，對拉曼探針分子具有好的檢測效率，因此，本實驗的拉曼檢測平台擁有巨大的潛力，相信未來可應用於許多的研究，如:生醫感測，食品安全等等。

Disease identification and prognosis are vital for disease assessment, prognosis, and treatment monitoring. The sensitive and rapid analysis capabilities of surface-enhanced Raman scattering (SERS) are widely used in various sensing technologies to identify analytes due to its ability to detect analytes at very low concentrations. In spite of this, developing a SERS substrate with fast recognition and stability remains a challenge. The objective of this work is to carbonize the zeolitic imidazolate framework-8 (ZIF-8) nanostructures through the use of a high temperature annealing process and modify the porous AuNR@Ag nanoparticles on the surface of nanoporous carbon nanostructures in order to obtain high SERS signals. The excitation wavelength of porous AuNR@Ag is adjusted to the laser excitation wavelength (632.8 nm) of the Raman spectroscope which leads to amplification and significant enhancement of the Raman signal. Consequently, the ZIF-8 derived nanoporous carbon decorated with plasmonic nanostructures has excellent Raman detecting efficiency. Therefore, our Raman sensing platform has huge potential and can be used for biomedical sensing, food safety and various research fields in the future.

目錄
致謝 2
摘要 3
圖目錄 9
表目錄 12
第一章 緒論 13
1.1引言 13
1.2研究動機 14
第二章 文獻回顧 15
2.1實驗運用之奈米材料 15
2.1.1 表面電漿子 (Surface plasmons, SPs) 15
2.1.2 金屬有機框架 (Metal organic framework, MOF) 16
2.2拉曼光譜學 17
2.2.1拉曼發展與簡介 17
2.2.2 拉曼散射機制 18
2.2.3表面增強拉曼散射(Surface-Enhanced Raman Scattering, SERS) 23
2.2.4表面增強拉曼散射機制(Surface Enhanced Raman Scattering Mechanism) 24
第三章 實驗方法與步驟 29
3.1實驗儀器 29
3.1.1 場發射掃描電子顯微鏡 (Field emission scanning electron microscope) 29
3.1.2 EDX能量色散X光譜分析儀 (Energy-dispersive X-ray spectrometer) 29
3.1.3 X射線繞射儀 (X-Ray Diffractometer) 29
3.1.4 紫外-可見分光譜儀（Ultraviolet–visible spectrometer，UV-Vis） 30
3.1.5 霍氏轉換紅外光譜儀 (Fourier-transform infrared spectrometer) 30
3.1.6 高解析電子能譜儀 (High resolution X-ray photoelectron spectrometer) 30
3.1.7感應耦合電漿質譜分析儀 (Inductively coupled plasma-mass spectrometer) 30
3.1.8 共軛聚焦顯微拉曼光譜儀 (Raman spectrometer) 31
3.1.9熱分析設備 (Thermal analyzers, TGA/DSC) 31
3.1.10高解像能穿透式電子顯微鏡 (Transmission electron micro-scope) 31
3.2實驗材料 32
3.2.1 實驗材料及化學品 32
3.3合成方法 33
3.3.1 棒狀金奈米結構(Gold nanorod, AuNR)的製程步驟 33
3.3.2 奈米棒狀之金銀核殼結構(Gold nanorod@silver, AuNR@Ag)合成 33
3.3.3 孔洞奈米棒狀之金銀核殼結構(Porous gold nanorod@silver, Porous AuNR@Ag)合成 33
3.3.4金屬有機框架ZIF-8(Zeolitic imidazolate framework-8, ZIF-8)的合成 34
3.3.5 ZIF-8衍生碳(ZIF-8 derived of carbon, NPC)的合成 34
3.3.6 透過真空抽氣過濾使NPC與奈米粒子沉積在濾紙 34
3.3.7 拉曼光譜測量 35
第四章 結果與討論 36
4.1 金/銀奈米結構的合成及材料分析 36
4.2 ZIF-8 和 ZIF-8 衍生碳的特性 40
4.3 表面電漿子奈米結構修飾於ZIF-8衍生的奈米多孔碳(NPC)應用於SERS檢測 43
4.4 表面電漿子奈米結構的吸附以增強拉曼效應 47
第五章 結論 57
第六章 參考文獻 58

圖目錄

圖 1. 拉曼效應之能態之能階圖55。 20
圖 2. 拉曼瑞利散射與拉曼散射(Stokes/ anti-Stokes)能階圖56。 21
圖 3. 共振拉曼光譜示意圖61。 22
圖 4. 局部表面電漿粒子共振 (Localized Surface Plasmon Resonance, LSPR) 示意圖。66,67從圖中顯示了傳導電子雲與原子核之間的相對位移。 25
圖 5. 位於聚乙二醇 (PEG) (8000 Da) 基質中銀奈米粒子熱點 (hot spot) 的示意圖68。從 (A) 和 (B) 中可以知道在顆粒連接處，有無熱點的形成，具有較長鏈的 (A)由於表面電漿共振所引起的電磁場的局部增加，將有助於分析物的表面增強拉曼散射 (SERS)；而 (B) 為較短鍊長 (1000 Da)，故無熱點產生，因此沒有得到拉曼增強訊號。 26
圖 6. 模擬兩金奈米粒子熱點圖中69。 27
圖 7. 分子-金屬複合物能階圖71。 28
圖 8. (a) AuNR, (b) AuNR@Ag, (c)具有Porous AuNR@Ag 的TEM 圖像。 (d) AuNR、AuNR@Ag 和具有孔洞結構 AuNR@Ag 的紫外-可見光-近紅外光譜。 37
圖 9. AuNR (a) (b)、AuNR@Ag (c) (d) 和具有孔洞結構的AuNR@Ag (e) (f)的長度和寬度統計圖。 38
圖 10. (a) AuNR@Ag 和(b)Porous AuNR@Ag 在基板上的 SEM 圖像。 (c) 在電置換反應期間添加不同體積的 HAuCl4 水溶液後 AuNR@Ag 的 UV-Vis-NIR 光譜。(c)中的虛線表示拉曼光譜的激發波長。 39
圖 11. 由 (a) 4、(b) 6、(c) 8、(d) 10 的各種Hmim/Zn摩爾濃度比製備的ZIF-8樣品的SEM圖像。 40
圖 12. ZIF-8和ZIF-8 衍生碳 (NPC)的SEM/TEM圖像。ZIF-8 的SEM圖像相對 (a) 低和 (b) 高放大倍率，(c) ZIF-8 的 TEM 圖像；ZIF-8 衍生碳 (NPC) 的 SEM 圖像，具有相對 (d) 低和 (e) 高放大倍率， (f) ZIF-8 衍生碳的 TEM 圖像。(c) 和 (f) 中的插圖是代表性為單個顆粒聚焦放大的 TEM 圖像。 41
圖 13. ZIF-8 衍生碳 (NPC) 和由 Hmim/Zn濃度摩爾相對比為4製備的 ZIF-8 樣品的元素圖譜分析 (EDX mapping) 42
圖 14. ZIF-8的熱比重分析 (TGA / DSC)。 43
圖 15. 表面電漿子奈米結構修飾的 ZIF-8 奈米多孔碳平台的工作原理示意圖。 43
圖 16. ZIF-8 和 ZIF-8 衍生碳的 XRD 和拉曼光譜分析。(a) (b) 分別為ZIF-8和ZIF-8 衍生碳 (NPC)的XRD 圖譜。 (c) (d) 分別為ZIF-8和ZIF-8 衍生碳 (NPC)的的拉曼光譜。 45
圖 17. ZIF-8 和 ZIF-8 衍生碳的 XPS分析。進行氧化態和表面化學成分，(a) ZIF-8 的 XPS全能譜圖掃描和 (b) 碳 (C1s)、(c) 氮 (N1s) 和 (d) 氧 (O1s) 的結合能。 (e) ZIF-8 衍生碳的 XPS全能譜圖掃描以及 (f) 碳 (C1s)、(g) 氮 (N1s) 和 (h) 氧 (O1s) ZIF-8 的結合能。 46
圖 18. ZIF-8 和 ZIF-8 衍生碳的 FTIR 光譜。 47
圖 19. ZIF-8在不同溫度下，高溫碳化的SEM圖。(a) 700°C (b) 900°C。 48
圖 20. ZIF-8衍生碳 (NPC) 表面吸附奈米粒子吸附聚集之SEM比較。(a)奈米粒子二次離心之後吸附及(b)奈米粒子經由一次離心後混和ZIF-8衍生碳 (NPC) 情況。 49
圖 21. ZIF-8衍生碳吸附於濾紙上情況。改善前後對比圖。 50
圖 22. 吸附ZIF-8衍生碳與奈米粒子紙於濾紙上示意圖。 51
圖 23. 浸泡於不同時間下，濾紙上的ZIF-8衍生碳的光學顯微鏡圖 (Optical microscope)。 52
圖 24. 於穩定持續之真空抽氣過濾下，在濾紙上滴入Porous AuNR@Ag示意圖。 53
圖 25. (a) 濾紙上有 ZIF-8 衍生碳 (NPC) 與Porous AuNR@Ag 的光學顯微鏡圖。(b) ZIF-8 衍生碳 (NPC) 表面吸附Porous AuNR@Ag 的 SEM 圖像。 (c) 在 100 pM 的固定 2-NT 濃度下，有或沒有Porous AuNR@Ag奈米顆粒增強，產生的 SERS 信號強度的差異。 (d) 2-NT 不同濃度梯度下的不同拉曼信號。 (a) 中的插圖是 SEM 圖像，比例尺為250 nm。 55
圖 26. 1381 cm-1 SERS峰的強度與2-NT濃度的關係。 56
 
表目錄

表 1. ICP-MS分析 40
表 2. BET孔隙分析檢測。 49

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