臺灣博碩士論文加值系統

本研究成功架設以冰晶法為主的水合物製作設備，可調整合成壓力，升降溫度曲線，以自行生產適合後續研究所需的水合物，並可同步紀錄製程中的壓力與溫度。添加乙醇做催化劑，縮短製程時間，加速實驗的進行。
嘗試裝填不同孔隙度的冰晶，合成出的水合物樣本也會有不同的孔隙度。實驗發現裝填的孔隙度越大，合成出的水合物孔隙度就越大，以顆粒大小180~250μm的冰晶來說，最大裝填孔隙度約為63.3~66.4%，合成出的水合物孔隙度約為46.62~51.1%；最小孔隙度約為51.8~55.8%，合成出得水合物孔隙度約為40.7~44.9%。
此外對合成出的水合物做一系列的檢測，如水合指數與甲烷釋放率測定等，結果顯示不同孔隙度的水合物在不同部位其水合指數基本一致，介於6.28~6.6之間(轉化率約為87~91%)，樣本整體有均勻之轉化率(轉化率相差在4%以內)。而單位面積與單位體積的甲烷釋放率與面體比有較大的關係，面體比越大，則單位面積與單位體積的甲烷釋放率越快
最後進行水合物的燃燒觀測，發現相同半徑的水合物，孔隙度越大者可以較快點燃，火焰也較快熄滅。而孔隙度接近的水合物，半徑越小者可以越早點燃，燃燒時間也較短。

The purpose of this study is to develop a standard procedure for artificially synthesize the methane hydrate with consistent and uniform properties for further observation and experiments of the combustion phenomena of methane hydrate. The synthesis procedure is based on ice-seed method, and adding the ethanol as the catalyst to shorten the processing time, if necessary.

By packing the ice-seed into different porosity, the synthesized hydrates will also have different porosity. With the larger porosity of the ice-seed, the porosity of the synthesized hydrates will also be greater. In this study, the grain size of the ice-seed is between 180~250μm. The largest packing porosity of ice-seed is between 63.3~66.4%, and the resultant porosity of synthesized hydrate is between 46.62~51.1%. The smallest packing porosity of ice-seed is between 51.8~55.8%, and the porosity of synthesized hydrate is between 40.7~44.9%.

Experimental results show that the hydration number of methane hydrate samples that synthesized by ice-seed method is between 6.28~6.6, the hydrate samples have a uniform conversion rate between 87~91%. In addition, the mass release rate of methane hydrate sample per unit area or unit volume can be related to the surface/volume ratio of the sample, the larger surface/volume ratio, the faster release rate of methane per unit area or unit volume.

Finally, the combustion phenomena of methane hydrate samples show that both the larger porosity of the methane hydrate sample with the same radius and the smaller radius of the methane hydrate sample with the same porosity can be ignited earlier with shorter ignition delay time and the flame extinguishes earlier with shorter flame lifespan.

摘要 I
Abstract III
致謝 XI
目錄 XII
表目錄 XVI
圖目錄 XVII
第一章緒論 1
1-1 天然氣水合物儲量與分布 1
1-2 水合物的基本性質 1
1-2-1 水合物結構 2
1-2-2 自保效應 4
第二章文獻回顧與研究動機 5
2-1 自然界水合物的開採方式 5
2-2 人工合成水合物 8
2-2-1 攪拌法 9
2-2-2 鼓泡法 10
2-2-3 噴霧法 10
2-2-4 冰晶法 11
2-2-5 添加沉積物或化學試劑法 12
2-3 水合指數及其檢測方式 13
2-4 以拉曼光譜檢測水合物 14
2-5 水合技術的應用 16
2-6 水合物燃燒研究 17
2-7 研究動機與目的 17
第三章實驗設備與研究方法 19
3-1 實驗設備 19
3-1-1 冰晶製作系統 19
3-1-2 增壓系統 20
3-1-3 高壓釜體 21
3-1-4 升降溫循環水槽 22
3-1-5 溫壓紀錄系統 22
3-1-6 拉曼光譜顯微鏡 23
3-1-7 冰盤 24
3-1-8 精密電子天秤 24
3-2 實驗流程 24
3-2-1 水合物製作流程 24
3-2-2 水合物拉曼光譜檢測流程 25
3-2-3 水合物甲烷釋放率測定 26
3-2-4 水合物燃燒流程 27
第四章結果與討論 28
4-1 以冰晶法製作水合物 28
4-1-1 冰晶製作 28
4-1-2 添加乙醇之合成結果 28
4-1-3 無預冷甲烷氣體 30
4-2 不同冰晶裝填孔隙度對合成後的水合物孔隙度影響 31
4-3 顯微拉曼光譜量測結果 31
4-4 水合物的甲烷釋放率 33
4-5 水合物燃燒 34
第五章結論與未來工作 39
5-1 結論 39
5-2 未來工作 40
參考文獻 42

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