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研究生： 陳煒澤
Chen, Wei-Ze
論文名稱： 聚乙烯亞胺-沸石咪唑骨架/多壁奈米碳管之雙層結構應用於室溫下人體呼氣二氧化碳感測
Application of Polyethylenimine-Zeolitic Imidazolate Framework/Multi-walled Carbon NanoTubes Bilayer Structure for Carbon Dioxide Gas Sensing from Human Breath at Room Temperature
指導教授： 戴念華
Tai, Nyan-Hwa
黃金花
Huang, Jin-Hua
口試委員: 李紫原
Lee, Chi-Young
彭殿王
Perng, Diahn-Warng
學位類別： 碩士
Master
系所名稱： 工學院 - 材料科學工程學系
Materials Science and Engineering
論文出版年： 2021
畢業學年度： 109
語文別： 中文
論文頁數： 106
中文關鍵詞： 奈米碳管 、沸石咪唑骨架 、聚乙烯亞胺 、氣體感測器 、二氧化碳
外文關鍵詞： carbon nanotube, zeolitic imidazolate framework, polyethylenimine, gas sensor, carbon dioxide
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    • 本研究製備了聚乙烯亞胺-沸石咪唑骨架/多壁奈米碳管(Polyethylenimine-
    Zeolitic imidazolate framework-8/Multi-walled carbon nanotubes, PEI-ZIF-8 /MWCNTs)之雙層材料，將其運用於人體呼氣之二氧化碳濃度監測，以應用於慢性肺阻塞病患者之病情監控及相關數據之收集。
    實驗上首先將MWCNT以噴塗法塗佈於網版印刷碳電極上，作為電子訊號傳輸層，接著合成PEI-ZIF-8複合材料，並再將其噴塗於電極上，運用PEI內富含胺基及ZIF-8的多孔特性，使其對於二氧化碳產生高量吸附之能力，當通入二氧化碳後電極之電阻會產生變化，以此做為判斷二氧化碳濃度之依據。本研究所製備之電極，在室溫環境、相對溼度10%的情況下，對於5 %濃度之二氧化碳(正常人呼氣之二氧化碳濃度)，可達5.29%之響應值(Response)，且在2.5%~12.5%之二氧化碳濃度區間內，訊號隨二氧化碳濃度增加呈現線性正相關之關係，顯示其對於二氧化碳濃度具有良好之判斷能力，在多次測試下也呈現穩定之響應訊號，在人體實際呼氣的狀況下也呈現良好的感測表現。
    本研究之電極及材料製備方法簡單、成本低廉，可直接於室溫環境下使用，且具有非侵入性、能簡易使用之特性，對於臨床醫學監測人體呼氣二氧化碳濃度之應用具極大的潛力。

    In this study, a polyethyleneimine-zeolitic imidazolate framework/multi-walled carbon nanotubes (PEI-ZIF-8/MWCNTs) double-layer electrode is prepared and applied to monitor the concentration of carbon dioxide (CO2) in human breath, aiming to monitor the physical health of patients with chronic obstructive pulmonary disease. In experiment, MWCNTs, used as the electron transport layer, are first coated on the screen-printed electrode by spray coating, and then the PEI-ZIF-8 solution is synthesized and sprayed on the electrode as the CO2 adsorption layer. The electrode with rich amine groups in PEI and the porous characteristics of ZIF-8 results in good ability to absorb CO2. The resistance varied in the presence of CO2 is used to determine the CO2 concentration. The sensor prepared in this work can reach an average response of 5.29% under 5% CO2 and 10% relative humidity at room temperature (RT). In addition, the response shows good linear relationship versus CO2 concentration in the range from 2.5% to 12.5%. In human breath test, the sensors also show good sensing behavior. The preparation of sensors and materials in this study are simple, low-cost, and the sensor possesses the characteristics of operation at RT, non-invasive and easy to use. The uniqueness of the electrode shows great potential for the application of clinical research to monitor the CO2 concentration of human breath.

    摘要 I Abstract II 致謝 III 目次 IV 表目次 IX 圖目次 X 第一章 緒論 1 1.1 前言 1 1.2 研究動機 3 第二章 文獻回顧 4 2.1 慢性肺阻塞病 4 2.1.1 慢性肺阻塞病之病理特徵 4 2.1.2 慢性肺阻塞病之檢測 7 2.1.3 人體呼氣檢測 9 2.2 奈米碳管簡介 10 2.2.1 奈米碳管之結構與性質 10 2.2.2 奈米碳管之製備方法 14 2.3 Zeolitic imidazolate framework-8 (ZIF-8) 簡介 18 2.3.1 ZIF-8之結構與性質 18 2.3.2 ZIF-8在氣體感測上之應用 20 2.4 Polyethylenimine (PEI) 簡介 22 2.4.1 PEI之基本性質 22 2.4.2 PEI 在氣體吸附上之應用 24 2.5 氣體感測器 26 2.5.1 不同種類之氣體感測器 26 2.5.2 奈米碳管感測器 28 2.5.3 奈米碳管感測器之改質 29 2.6 本實驗室在氣體感測研究之回顧 33 第三章 實驗方法與分析 35 3.1 實驗製備 35 3.1.1 實驗藥品 35 3.1.2 網版印刷電極 38 3.1.3 奈米碳管之酸處理 38 3.1.4 ZIF-8之合成 40 3.1.5 PEI-ZIF-8之合成 40 3.1.6 奈米碳管於電極上之塗佈 41 3.1.7 感測材料於電極上之塗佈 41 3.2 實驗製程設備 41 3.2.1 電磁加熱攪拌器 41 3.2.2 水循環抽濾器 42 3.2.3 高速離心機 42 3.2.4 超音波震盪器 42 3.2.5 高速超音波震盪棒 43 3.2.6 噴塗槍 43 3.2.7 自動噴塗系統 43 3.3 材料分析儀器 45 3.3.1 Ｘ光繞射儀 45 3.3.2 場發射掃描式電子顯微鏡 46 3.3.3 拉曼光譜儀 47 3.3.4 傅立葉轉換紅外光譜儀 47 3.3.5 比表面積分析儀暨孔隙分析儀 48 3.3.6 Ｘ射線光電子能譜儀 51 3.3.7 原子力顯微鏡 51 3.3.8 穿透式電子顯微鏡 51 3.4 氣體感測系統 54 3.4.1 氣體感測系統的架構 54 3.4.2 二氧化碳濃度之計算 54 3.4.3 感測響應值之計算 55 3.4.4 模擬室溫下二氧化碳濃度感測之操作流程 57 第四章 結果與討論 59 4.1 酸處理奈米碳管分析 59 4.1.1 X光繞射光譜分析 59 4.1.2 拉曼光譜儀鍵結分析 61 4.1.3 傅立葉轉換紅外光譜分析 61 4.1.4 掃描電子顯微鏡分析 63 4.1.5 穿透式電子顯微鏡分析 65 4.2 ZIF-8/PEI-ZIF-8結構成分分析 67 4.2.1 X光繞射光譜分析 67 4.2.2 傅立葉轉換紅外光譜分析 68 4.2.3 掃描式電子顯微鏡之形貌分析 69 4.2.4 比表面積分析 71 4.2.5 穿透式電子顯微鏡分析 77 4.3 感測電極逐層分析 79 4.3.1 X光繞射光譜分析 79 4.3.2 掃描電子顯微鏡之形貌分析 81 4.3.3 X射線電子能譜儀分析 83 4.3.4 原子力顯微鏡分析 85 4.4 室溫環境下之二氧化碳感測 87 4.4.1 單次循環感測分析 87 4.4.2 逐層材料對感測效能影響之分析 89 4.4.3 噴塗參數對感測效能影響之分析 90 4.4.4 不同濃度CO2感測分析 91 4.4.5 電極穩定性分析 93 4.4.6 濕度環境及人體呼氣感測分析 95 4.4.7 二氧化碳氣體感測之可能機制 97 第五章 結論 99 第六章 參考文獻 100

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