臺灣博碩士論文加值系統

本研究採用一套高壓設備，並採用等容溫度循環法，進行二氧化碳水合物之熱力學與動力學實驗。目的在於測量含有化學添加劑的二氧化碳水合物之熱力學相平衡數據，以及二氧化碳水合物生成的動力學數據，以作為未來工程設計、探採與操作的基礎資料。本研究所選用之添加劑為N-甲基吡咯烷酮及N-甲基嗎啉。

本研究之實驗結果顯示，添加N-甲基吡咯烷酮對於二氧化碳水合物的生成有熱力學上抑制之效果，使二氧化碳水合物的相平衡曲線往低溫高壓的方向移動，其抑制效果在30 wt% N-甲基吡咯烷酮時最大，可減少平衡溫度約6.1 K。而添加N-甲基嗎啉對於二氧化碳水合物亦為熱力學上抑制的效果，在20 wt% 時可降低平衡溫度約5.7 K。此外，為了模擬添加劑在海洋環境中的效果，本研究進行二氧化碳＋鹽水＋添加劑之水合物系統相平衡量測，實驗結果發現添加N-甲基吡咯烷酮及N-甲基嗎啉皆使二氧化碳水合物相平衡曲線往更低溫和更高壓的方向移動。

在熱力學實驗過程中，觀察發現添加N-甲基吡咯烷酮之二氧化碳水合物系統，其在動力學上具有促進水合物生成的效果，故本研究以N-甲基吡咯烷酮為添加劑進行動力學實驗。由實驗之結果證實，相較於純水系統而言，添加N-甲基吡咯烷酮可縮短水合物生成之誘導時間並增加水合物之生成量。

摘要 I
Abstract II
目錄 IV
表目錄 VI
圖目錄 VIII
第一章 緒論 1
1-1 水合物簡介 2
1-2 二氧化碳捕捉與封存 4
1-3 二氧化碳水合物介紹及應用 7
1-4 研究方向與目的 9
第二章 文獻回顧 11
2-1 水合物相律及相圖 11
2-2 水合物形成機制 13
2-3 水合物之熱力學研究 14
2-4 水合物之動力學研究 17
2-5 水合物之結構鑑定 19
第三章 實驗方法 21
3-1 實驗設備與藥品 22
3-2 實驗步驟 23
3-2.1 熱力學實驗步驟 23
3-2.2 動力學實驗步驟 25
3-3 實驗數據分析 27
3-3.1 熱力學實驗數據分析 27
3-3.2 動力學實驗數據分析 28
第四章 結果與討論 29
A. 二氧化碳水合物之熱力學相平衡實驗 29
4A-1 溫度循環流程之討論 29
4A-2 二氧化碳水合物之對比實驗量測 30
4A-3 化學添加劑之篩選及快速溫度循環測試實驗 32
4A-4 二氧化碳+純水+ N-甲基吡咯烷酮之水合物系統相平衡實驗 34
4A-4.1 二氧化碳+純水+N-甲基吡咯烷酮之水合物相平衡數據 34
4A-4.2 二氧化碳+純水+N-甲基吡咯烷酮之水合物結構預測 35
4A-5 二氧化碳+純水+ N-甲基嗎啉之水合物系統相平衡實驗 35
4A-5.1 二氧化碳+純水+ N-甲基嗎啉之水合物相平衡數據 35
4A-5.2 二氧化碳+純水+ N-甲基嗎啉之水合物結構預測 36
4A-6 N-甲基吡咯烷酮與 N-甲基嗎啉之添加劑討論 36
4A-7二氧化碳+鹽水+添加劑之水合物系統相平衡實驗 38
4A-7.1 二氧化碳+鹽水+添加劑之水合物相平衡數據 38
4A-7.2 二氧化碳+鹽水+添加劑之水合物結構預測 39
B. 二氧化碳水合物之動力學實驗 41
4B-1 動力學升壓實驗流程之討論 41
4B-2 動力學實驗操作條件之選擇 42
4B-3 動力學實驗結果討論 43
4B-3.1 二氧化碳水合物系統之添加劑效應探討 43
4B-3.2 二氧化碳+純水+N-甲基吡咯烷酮系統之過冷溫度探討 44
4B-3.3 二氧化碳+純水+N-甲基吡咯烷酮系統之操作壓力探討 45
第五章 結論 47
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