臺灣博碩士論文加值系統

第一部分
本研究中利用沸石咪唑結構材料(ZIF-67)的特性開發作為對乙酰氨基酚的感測器和比色法奈米酶的複合材料。ZIF-67主要透過三種不同的製備方法合成ZIF-67-C、ZIF-67-A 和 ZIF-67-H。接著透過使用X光繞射儀、高解析度場發射掃描式電子顯微鏡、穿透式電子顯微鏡進行表徵分析證實所合成的材料具有增加電催化活性的菱形十二面體結構。ZIF-67-C做為奈米酶時，所表現的電子親和力明顯高過於ZIF-67-A和ZIF-67-H。而 ZIF-67-A 和ZIF-67-H 與ZIF-67-C相比時，因為晶體排列和結晶較不完善導致對乙酰氨基酚檢測的性能較低。在河水以及湖水中的真實樣品下，我們針對乙酰氨基酚去做感測結果顯示該感測器在這兩種樣品中都出了具有良好的感測率。其中製備的ZIF-67-C樣品的高表面積、導電性、高孔隙率有利於雙感測應用，並確定可用於多種應用。
第二部分
本章節中，透過簡單方法合成氧化銅與氧化鋅複合材料(CZ)並開發作為對尼美舒利(NMS)的感測器，且透過使用X光繞射儀和高解析度場發射掃描式電子顯微鏡進行表徵分析並觀察出CZ的高度結晶性，且具有CZ的2D奈米薄片的行程。在使用CZ修飾的玻璃碳電極上，對NMS的電化學感測反應了更高的電催化性，添加的縣性範圍為0.299 µM 至 319.15 µM，檢測極限約為0.005µM，靈敏度約為7.152 µAµM-1 cm-2。CZ奈米複合材料與高導電材料的金屬氧化物相比，更適用於檢測具有豐富的活性位、高電導率、高表面積的藥物。
第三部分
我們製造了氧化鎳/氧化鋅 (NZ) 雙金屬氧化物複合材料並修飾在玻璃碳電極的表面，並將其用於檢測有害物質化合物蘆丁 (RT)。透過使用X光繞射儀、高解析度場發射掃描式電子顯微鏡、穿透式電子顯微鏡進行表徵分析，證實了NZ材料的成功形成。此外，NiO/ZnO/GCE具有更高的電子傳輸率和404 Ω電荷轉移電阻來體現出色的動力學性質。所提出的NiO/ZnO/GCE感測器在可行性分析上具有好的選擇性、再現性、儲存穩定性。最重要的是在血液和柳橙的即時監測分析上其回收結果相當精確。

First part:
The outgrowth of the zeolitic imidazole framework (ZIF-67) with substantial benefits was significantly used in the present study. The attractive properties of ZIF-67 are envisioned to develop a dual-functionalsensing platform as electrochemical and colorimetric for acetaminophen detection. Co-ZIF-67 wasdeveloped as a synthesis-controlled material via three different preparation techniques as ZIF-67-C, ZIF-67-A, and ZIF-67-H. ZIF-67-C prepared via simple co-precipitation strategy in room temperature ac-quired rhombic dodecahedral structure with increased electrocatalytic activity. ZIF-67-C nanozyme ex-hibits enzymatic activity with intrinsic peroxidase mimicking and higher electron affinity than ZIF-67-Aand ZIF-67-H. The well-developed ZIF-67-C without further aggregation and a steadily build structure resulted in an enhanced response. While the higher chance of aggregation and irregular arrangements ofZIF-67-A and ZIF-67-H resulted in lower performance toward acetaminophen detection. Moreover, theabsorption of Tetramethylbenzidine (TMB) molecules could lower the diffusion distance leading to improved peroxidase mimicking activity.
Second part:
This simple and cost-effective development of the CZ composite was characterized for evaluating the physical, chemical, and morphological properties. The highly crystalline nature of CZwas observed from powder X-ray diffraction and X-ray photoelectron spectroscopy analysis. The formation of 2D nanoflakes of CZ was strongly confirmed from field emission scanning electron microscopy and high-resolution transmission electron microscopy images. To verify the strong attachments, Fourier transforms infrared spectroscopy spectra were analyzed. Electrochemical sensing of NMS at CZ fabricated glassy carbon electrode reflects higher electrocatalytic activity with a linear range of NMS addition from 0.299 µM to 319.15 µM. The lower detection limit was about 0.005 µM with a sensitivity of 7.152 µAµM-1 cm2. The CZ nanocomposite will be more applicable for sensing several drugs with enriched active sites, higher conductivity, and large surface area raised fromlowcost metal oxides when compared with highly conducting materials.
Third part
We fabricated Nickel oxide/Zinc Oxide (NiO/ZnO) binary metal oxide composite on the superficial region of GCE and implemented it towards electrochemical detection of hazardous flavoring compound Rutin (RT). The successful formation of Nickel oxide/Zinc Oxide (NiO/ZnO) composite has been scrutinized through various microscopic and spectroscopic techniques. Further, NiO/ZnO/GCE tends to exemplify exquisite kinetic performance with a higher electron transfer rate and charge transfer resistance (Rct) of 404 Ω. The practical feasibility analysis of a proposed NiO/ZnO/GCE sensor features exemplary selectivity, repeatability, reproducibility, and storage stability. On top of that, the real-time monitoring analysis demonstrates exquisite recovery results in blood and orange samples.

摘要 i
ABSTRACT iii
目錄 vi
表目錄 ix
圖目錄 x
1 第一章 緒論 1
1.1 電化學分析簡介 1
1.2 感測器簡介 2
1.3 電極簡介 4
1.3.1 化學修飾電極 4
1.4 藥品簡介 5
1.4.1 對乙醯胺基酚(Acetaminophen) 5
1.4.2 黃酮(Flavonoids) 6
1.4.3 尼美舒利(Nimesulide) 6
2 第二章 實驗藥品、器材與分析方法 8
2.1 實驗藥品 8
2.2 實驗器材 9
2.3 分析方法 9
2.3.1 循環伏安法(Cyclic Voltammetry, CV) 9
2.3.2 微分脈衝伏安法 (Differential Pulse Voltammetry, DPV) 10
2.3.3 安培法(Amperometry) 11
2.3.4 電化學阻抗譜法(Electrochemical Impedance Spectroscopy，EIS) 12
2.3.5 掃描式電子顯微鏡(Scanning Electron Microscope, SEM) 13
2.3.6 X-射線繞射分析儀（X-ray diffractometer，XRD） 14
2.3.7 穿透式電子顯微鏡(Transmission Electron Microscope, TEM) 15
2.3.8 比表面積與孔隙度分析儀(Specific Surface Area & Pore Size Distribution Analyzer) 16
2.3.9 X射線光電子光譜法(X-ray photoelectron spectroscopy, XPS) 16
3 第三章 18
3.1 前言 18
3.2 實驗步驟 21
3.2.1 ZIF-67奈米薄片合成 21
3.2.2 製備ZIF-67奈米薄片修飾電極 21
3.2.3 真實樣品的製備 21
3.3 結果與討論 22
3.3.1 ZIF-67奈米薄片特徵分析 22
3.3.2 ZIF-67/GCE電化學特性分析 24
3.3.3 不同參數對ZIF-67-C修飾電極之影響 25
3.3.4 ZIF-67-C/GCE以微分脈衝伏安法(DPV)對ACM感測分析 28
3.3.5 穩定性、再現性、可重現性與真實樣品分析 30
3.4 比色法檢測ACM 33
3.4.1 研究ZIF-67-C的過氧化酶 33
3.4.2 ZIF-67-C過氧化酶催化活性的動力學分析 34
3.5 結論 36
4 第四章 37
4.1 前言 37
4.2 實驗步驟 39
4.2.1 氧化銅/氧化鋅奈米薄片(CZ)的合成 39
4.2.2 氧化銅/氧化鋅奈米薄片(CZ)修飾電極的製備 40
4.3 結果與討論 40
4.3.1 氧化銅/氧化鋅(CZ)奈米薄片特徵分析 40
4.3.2 CZ/GCE電化學特性分析 44
4.3.3 CZ/GCE對尼美舒利(NMS)的電化學感測 45
4.3.4 CZ/GCE以微分脈衝伏安法(DPV)對NMS感測分析 49
4.3.5 穩定性、再現性、可重現性與真實樣品分析 50
4.4 結論 54
5 第五章 56
5.1 前言 56
5.2 實驗步驟 58
5.2.1 NiO/ZnO(NZ)奈米薄片合成 58
5.2.2 真實樣品的製備 58
5.2.3 NiO/ZnO修飾電極製備 58
5.3 結果與討論 59
5.3.1 氧化鎳/氧化鋅與氧化鋅奈米薄片特徵分析 59
5.3.2 ZnO/GCE和NiO/ZnO/GCE電化學特性分析 61
5.3.3 NiO/ZnO/GCE對芸香苷(RT)的電化學感測 62
5.3.4 NiO/ZnO/GCE以微分脈衝伏安法(DPV)對RT感測分析 64
5.3.5 穩定性、再現性、可重現性與真實樣品分析 64
5.4 結論 67
參考文獻 68

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