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系統識別號 U0026-0707202019234900
論文名稱(中文) 含浸法摻入石墨烯量子點於金屬有機骨架以提升導電性及電化學感測活性
論文名稱(英文) Impregnation of Graphene Quantum Dots into a Metal–Organic Framework to Render Increased Electrical Conductivity and Activity for Electrochemical Sensing
校院名稱 成功大學
系所名稱(中) 化學工程學系
系所名稱(英) Department of Chemical Engineering
學年度 108
學期 2
出版年 109
研究生(中文) 陳昱全
研究生(英文) Yu-Chuan Chen
學號 N36071447
學位類別 碩士
語文別 中文
論文頁數 99頁
口試委員 指導教授-龔仲偉
口試委員-江偉宏
口試委員-王誠佑
中文關鍵字 導電金屬有機骨架  施體-受體電子傳輸  電催化  電化學感測  亞硝酸鹽氧化  以鋯為基底之金屬有機骨架 
英文關鍵字 conductive MOF  donor−acceptor charge transfer  electrocatalysis  electrochemical sensor  mesoporous  nitrite oxidation  zirconium-based MOF 
學科別分類
中文摘要 金屬有機骨架(MOFs),因為結構多樣性、功能可調節性、較高的比表面積和永久的孔隙率,在過去的二十年中引起了相當大的關注。而MOFs目前已被廣泛應用在各種領域,例如氣體儲存、催化、化學分離和化學感測器。但是大多數MOFs在水相環境中有著較差的穩定性和較低導電度,這也限制了它們在許多應用中的發展。然而以鋯為基底MOF(Zr-MOF)通常在水相中穩定,因此近年來已被廣泛使用在許多應用上,但是導電Zr-MOF的例子仍然非常少見。
石墨烯量子點(GQDs)為奈米片狀石墨,具有高穩定性、好的生物相容性、優異的分散性和容易調控尺寸的優勢,透過調控尺寸造成量子侷限效應以調控其電子結構。本研究藉由含浸法將平均大小為3.1奈米GQDs摻入於以卟啉及鋯為基底的中孔金屬有機骨架中,以呈現施體-受體電子傳遞從石墨烯量子點傳遞到有機連接器卟啉。由實驗結果可知,製備出的複合材料導電性提升了超過一百倍且還具有一半的孔洞性。而有機連接器卟啉可作為電觸媒用於感測亞硝酸鹽,比較安裝GQD前後的金屬有機骨架之電化學感測表現,安裝GQD後其電化學感測效果更為優異。
英文摘要 Graphene quantum dots (GQD) with an average size of 3.1 nm were incorporated into a mesoporous porphyrinic zirconium-based metal–organic framework (MOF) by direct impregnation to render the donor–acceptor charge transfer from GQDs to porphyrinic linkers. The hybrid material still possesses around half porosity of the pristine MOF and shows a 100-fold higher electrical conductivity compared to that of the parent MOF. By utilizing the porphyrinic linkers as catalytically active units, the GQD-MOF material exhibits a better electrochemical sensing activity toward nitrite in aqueous solutions compared to both the pristine MOF and GQD. The linear range of the hybrid material for the determination of nitrite is 40-18000 μM. and the limit of detection is 6.4 μM.
論文目次 中文摘要 I
Extended Abstract II
誌謝 X
目錄 XI
表目錄 XV
圖目錄 XVI
第一章 緒論 1
1-1前言 1
1-2 電化學介紹 3
1-2-1 電化學簡介 3
1-2-2 電極簡介 4
1-2-3 修飾電極簡介 5
1-3 電化學感測 8
1-3-1 電位式感測(Potentiometric sensor) 10
1-3-2 電流式感測(Amperometric sensor) 10
1-3-3 電阻式感測(Impedimetric sensor) 12
1-4 電流式感測亞硝酸鹽觸媒 13
1-5 金屬有機骨架與其於電化學感測之應用 16
1-5-1 金屬有機骨架介紹 16
1-5-2 金屬有機骨架水穩定性與導電性提升 19
1-5-3 金屬有機骨架於電化學感測亞硝酸鹽應用 25
1-6 材料簡述 30
1-6-1 石墨烯量子點(Graphene quantum dot) 30
1-6-2 金屬有機骨架:PCN-222 31
1-7 研究動機 33
第二章 實驗方法與儀器原理介紹 34
2-1 藥品、材料與儀器設備 34
2-1-1 藥品與材料 34
2-1-2 儀器與實驗設備 35
2-2 儀器原理介紹 36
2-2-1 掃描式電子顯微鏡(Scanning electron microscope, SEM)
36
2-2-2 X射線繞射儀(X-ray diffractometer, XRD) 36
2-2-3 等溫氮氣吸/脫附儀 (Accelerated surface area and porosimetry system ) 37
2-2-4 光致螢光光譜儀(Photoluminescence, PL) 38
2-2-5 循環伏安法(Cyclic voltammetry, CV) 39
2-2-6 電化學阻抗圖譜(Electrochemical impedance spectroscopy, EIS) 40
2-3 實驗方法 41
2-3-1 石墨烯量子點(GQD)製備 41
2-3-2 金屬有機骨架PCN-222製備 42
2-3-3 GQD-PCN-222複合材料製備 43
2-3-4 錠片和薄膜製備 44
第三章 結果與討論 46
3-1 材料鑑定 46
3-2 電化學結果分析 61
3-2-1 循環伏安分析 61
3-2-2 交流阻抗分析 65
3-2-3 電流式感測分析 67
3-2-4 材料穩定度測試 73
3-2-5 干擾物測試 74
第四章 結論 75
第五章 未來展望與建議 77
參考文獻 79
附錄:個人履歷表 96
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