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研究生: 陳鴻博
Chen, Hong-Po
論文名稱: 以中孔氧化石墨烯奈米粒子結合表面輔助雷射游離/脫附檢測精神活性物質
Detection of Psychoactive Substances by Using Mesoporous Graphene Oxide Nanoparticles with Surface-Assisted Laser Desorption/Ionization
指導教授: 劉沂欣
Liu, Yi-Hsin
口試委員: 葉怡均
Yeh, Yi-Chun
陳珮珊
Chen, Pai-Shan
劉沂欣
Liu, Yi-Hsin
口試日期: 2023/07/27
學位類別: 碩士
Master
系所名稱: 化學系
Department of Chemistry
論文出版年: 2023
畢業學年度: 111
語文別: 中文
論文頁數: 93
中文關鍵詞: 中孔洞沸石奈米粒子氧化石墨烯基質輔助雷射游離/脫附表面輔助雷射游離/脫附精神活性物質濫用藥物
英文關鍵詞: mesoporous zeolite nanoparticles, graphene-oxide, MALDI-TOF MS, SALDI-TOF MS, Psychoative Substances, abuse drugs
研究方法: 實驗設計法
DOI URL: http://doi.org/10.6345/NTNU202301556
論文種類: 學術論文
相關次數: 點閱:104下載:4
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  • 本研究以中孔氧化石墨烯奈米粒子 (mesoporous graphene oxide nanoparticles, MGNs) 作為新型奈米基質,結合表面輔助雷射游離脫附 (surface-assisted laser desorption/ionization, SALDI) 技術檢測精神活性物質,提升表面質譜檢測之再現性及低荷質比區間 (m/z 100-500) 背景干擾問題。類似於中孔洞沸石奈米粒子 (MZNs) 具有高比表面積 (>900 m2/g) 及孔洞 (5-6 nm) 之高孔容 (≈1 mL/g) 具有優異的吸附藥物能力,MGNs表面因具有氧化石墨烯的強吸光性 (200-900 nm) 及近紅外放光 (1000-2500 nm) 特性,具有優異的光熱轉換效率提供精神活性物質游離/脫附之能量。對照兩種有機酸-基質龍膽酸 (2,5-Dihydroxybenzoic acid, DHB) 、α-氰基-4-羥基肉桂酸 (α-cyano-4-hydroxycinnamic acid, α-CHCA) 和商業化氧化石墨烯 (GO) 檢測精神活性物質的質譜結果,MGNs偵測濃度已達到法規濃度 (50 ppb) 等級且具有更低的背景訊號,且對於真實樣品之定量誤差值小於10%。此外,透過結合自動化技術分離尿液與咖啡包檢體,有望達到即時輔助臨床檢測進行毒癮即時檢測及防治。

    In this study, mesoporous graphene oxide nanoparticles (MGNs) were used as a new nano-matrix, combined with surface-assisted laser desorption/ionization (SALDI) technology to detect psychoactive substances. Improve the reproducibility of surface mass spectrometry detection and the background interference problem in the low charge-to-mass ratio range (m/z 100-500). Similar to mesoporous zeolite nanoparticles (MZNs), it has a high specific surface area (>900 m2/g) and a high pore volume (≈1 mL/g) of pores (5-6 nm) with excellent ability to adsorb drugs. The surface of MGNs has Graphene oxide has strong light absorption (200-900 nm) and near-infrared light emission (1000-2500 nm) characteristics, and has excellent photothermal conversion efficiency to provide energy for the dissociation/desorption of psychoactive substances. Comparison of two organic acids-matrix gentisic acid (2,5-Dihydroxybenzoic acid, DHB), α-cyano-4-hydroxycinnamic acid (α-cyano-4-hydroxycinnamic acid, α-CHCA) and commercial graphite oxide The mass spectrometry results of GO detection of psychoactive substances, the detection concentration of MGNs has reached the legal concentration (50 ppb) level and has lower background signals, and the quantitative error value for real samples is less than 10%. It is also possible to separate urine and coffee bag samples by combining automation technology, which is expected Achieve real-time auxiliary clinical detection for real-time detection and prevention of drug addiction.

    謝誌 i 摘要 ii Abstract iii 目錄 iv 圖目錄 vii 表目錄 xii 第一章 緒論 1 1.1 精神活性物質類型與分析挑戰性 1 1.1.1 精神活性物質概述 1 1.1.2 流行率和影響 3 1.1.3 現有分析方法及其挑戰性 3 1.2 表面輔助雷射脫附游離概述 5 1.2.1 MALDI-MS簡介及小分子分析 5 1.2.2 SALDI-MS簡介及小分子分析 8 1.3 中孔洞氧化石墨烯 10 1.4 研究目的與動機 12 第二章 實驗方法 13 2.1 化學藥品 13 2.2 沸石晶種合成 (beta zeolite seed, BZS) 15 2.3 中孔洞奈米粒子合成 16 2.3.1 中孔沸石奈米粒子 (MZNs) 16 2.3.2 中孔洞氧化石墨烯奈米粒子之合成 (MGNs) 17 2.4 中孔洞負載銀奈米粒子之合成 (Ag@MZNs) 18 2.4.1 表面官能基化修飾 18 2.4.2 銀前驅物之吸附 18 2.4.3 銀奈米粒子還原 19 2.5 磁性氧化石墨烯之合成 (Fe-MGNs/GO) 19 2.6 MALDI質譜校正與樣品備製 20 2.6.1 標準品備製 20 2.6.2 真實檢體製備 20 2.6.2.1 咖啡包樣品製備 20 2.6.2.2 尿液樣品製備 20 2.6.3 MALDI質譜校正與QC 21 2.6.4 MALDI質譜量測條件 21 2.7 材料合成及鑑定儀器 22 2.7.1 化學氣相沉積儀 (chemical vapor deposition, CVD) 22 2.7.2 反射式紫外-可見光光譜儀 (diffused reflectance ultraviolet–visible spectroscopy, DRS) 23 2.7.3 拉曼光譜儀 (Raman spectrometer) 23 2.7.4 比表面積及孔徑分析儀 (Brunauer-Emmett-Teller, BET) 24 2.7.5 介面電位分析儀 (zeta potential analyzer) 24 2.7.6 穿透式電子顯微鏡 (transmission electron microscopy, TEM) 25 2.7.7 元素分析儀 (Elemental Analyzer, EA) 25 2.7.8 基質輔助雷射脫附游離飛行時間式質譜儀 (Matrix-assisted laser desorption ionization-time of flight Mass Spectrometry, MALDI-TOF-MS) 25 2.7.9 衰減式全反射傅立葉轉換红外線光譜(Attenuated Total Reflection Fourier-Transform Infrared Spectrometer, ATR-FTIR) 26 2.7.10 X光粉末繞射儀 (powder X-ray diffraction, PXRD) 27 第三章 結果與討論 28 3.1 最佳化之基質選擇 28 3.1.1 有機酸基質 28 3.1.2 固體酸碳基質 31 3.1.3 無機孔洞材料基質 33 3.2 無機孔洞複合材料之鑑定 37 3.2.1 形貌及孔洞性質 37 3.2.2 其他性質 41 3.3 表面輔助雷射脫附/游離檢測條件優化 46 3.3.1 儀器參數之優化 46 3.3.2 備製方法之比較探討 51 3.3.3 化學表面修飾之比較探討 61 3.3.3.1 氧化石墨烯複合材料 61 3.3.3.2 磁性複合材料 70 3.4 檢體分析及方法確效 73 3.4.1 MALDI/SALDI建立校正曲線 73 3.4.2 真實檢體 79 3.4.3 自動化分離系統 82 第四章 結論與未來展望 86 參考文獻 87

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