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研究生： 劉泓柜
Liou, Hong-Jyu
論文名稱： 甲烷催化裂解於傳統加熱與微波加熱環境中氫氣生成之建模與數值模擬
Modeling and Simulation of Methane Thermocatalytic Decomposition in Conventional Heating and Microwave Heating for Hydrogen Production
指導教授： 洪振益
Hung, Chen-I
學位類別： 碩士
Master
系所名稱： 工學院 - 機械工程學系
Department of Mechanical Engineering
論文出版年： 2013
畢業學年度： 101
語文別： 中文
論文頁數： 94
中文關鍵詞： 數值方法 、產氫 、甲烷催化裂解 、傳統加熱 、微波加熱 、建模
外文關鍵詞： Numerical simulations, Hydrogen production and generation, Thermocatalytic decomposition (TCD) of methane, Conventional heating, Microwave heating, Modeling
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    • 本研究建立甲烷催化裂解產氫之動力模型，數值模擬可以清楚提供在觸媒床之詳細的反應現象。甲烷催化裂解為一個無CO與CO2生成之產氫方式。本研究區分為兩部分，一個為傳統加熱下之甲烷催化裂解，另一個為微波加熱下之甲烷催化裂解。第一部分的研究中分別建立傳統加熱下甲烷催化裂解產氫初期階段與穩定狀態兩種化學反應動力式模型，接著探討反應（壁面）溫度、觸媒質量、以及反應物流率對甲烷催化裂解之影響，從模擬預測得知在初期階段甲烷轉化率與反應溫度呈現一個線性比例。而在穩定狀態化學反應對於溫度較為敏感，而且流速對於產氫的反應也有一定的影響，相反地，相較此兩狀態下觸媒質量對甲烷催化裂解反應的影響相對的小，從觸媒床內溫度、化學反應速率以及氫濃度可以得知，化學反應為二維分布，溫度與濃度幾乎是一維分布。
    在第二部分中，為了清楚了解微波輻射與甲烷催化裂解於活性碳觸媒床下之交互作用，以數值方式建構微波輔助加熱甲烷催化裂解之物理模型，微波輔助加熱下影響甲烷催化裂解有兩個重要參數，分別是提供之功率與體時空速（VHSV），從模擬結果得知提供更高的功率可以有效的促進甲烷催化裂解的表現，雖然增加體時空速甲烷轉化率會降低，但產氫量會增加。

    Chemical kinetics of hydrogen production from the thermocatalytic decomposition (TCD) of methane is modeled in this study. Numerical simulations are carried out to figure out the detailed reaction phenomena in a catalyst bed. TCD of methane is a noticeable route to produce hydrogen without the formation of CO and CO2. This study is separated into two parts. One is TCD of methane with conventional heating, and the other is TCD of methane with microwave heating. At the first part, chemical kinetics of hydrogen production from the TCD of methane at the early reaction stage and the steady state with conventional heating is modeled. The effects of reaction (wall) temperature, catalyst mass, and reactant flow rate on the performance of methane TCD are evaluated. The predictions suggest that the CH4 conversion is linearly proportional to the reaction temperature at the early stage; the reaction is more sensitive to the reaction temperature at the steady state. Hydrogen formation from the reaction is also affected by the flow rate to a certain extent. In contrast, the performance of methane TCD is relatively insensitive to the catalyst mass, regardless of which reaction stage is. When the temperature distribution, reaction rate, and H2 concentration in the catalyst bed are examined, two-dimensional contours of reaction rate are exhibited, whereas the isothermal and concentration contours are almost one-dimensional.
    At the second part, to recognize the characteristics of interaction of methane TCD and microwave irradiation in an activated carbon catalyst bed, the chemical reaction along with microwave-assisted heating is modeled and simulated numerically. The influences of two important factors, namely, the supplied power and volumetric hourly space velocity (VHSV), on the performance of methane TCD are investigated. The predictions suggest that a higher power supply can efficiently promote the performance of methane TCD. Increasing VHSV reduces the CH4 conversion, but more hydrogen is produced.

    摘要 II 誌謝 VI 目錄 VII 表目錄 XI 圖目錄 XII 符號說明（Nomenclature） XV 第一章 緒論 1 1.1 前言 1 1.2 研究動機及目的 5 1.3 研究流程圖 7 第二章 文獻回顧 8 2.1 甲烷催化裂解反應 8 2.2 微波加熱（Microwave heating） 12 2.3 現有之化學反應結合微波加熱之研究 17 第三章 研究方法 20 3.1 物理問題及模式說明 20 3.2 模型問題之基本假設 20 3.3 傳統加熱之物理模型 22 3.3.1 統御方程式（Governing equations） 22 3.3.1.1 非多孔隙區域之統御方程式（Governing equations of non-porous region） 22 3.3.1.2 多孔隙區域之統御方程式（Governing equations of porous region） 23 3.3.2 邊界條件設定 25 3.3.3 甲烷催化裂解反應機制 27 3.3.4 混合氣之性質 27 3.3.4.1 黏滯係數（Viscosity） 28 3.3.4.2 熱傳導係數與比熱（Thermal conductivity and specific heat） 29 3.3.4.3 擴散係數（Diffusion coefficient） 29 3.4 微波加熱之物理模型 33 3.4.1 統御方程式（Governing equations） 33 3.4.1.1 非多孔隙區域之統御方程式（Governing equations of non-porous region） 33 3.4.1.2 多孔隙區域之統御方程式（Governing equations of porous region） 34 3.4.1.3 微波加熱項 37 3.4.2 邊界條件設定 37 3.4.3 甲烷催化裂解反應機制 38 3.5 數值方法（Numerical method） 39 3.5.1 離散（Discretization） 40 3.5.2 SPOOLES求解 41 3.5.3 GMRES求解 41 3.5.4 阻尼常數（Damping constant） 42 3.5.5 收斂標準 42 3.6 格點獨立性測試 42 3.6.1 傳統加熱之格點獨立測試 42 3.6.2 微波加熱之格點獨立測試 44 第四章 結果與討論 46 4.1 傳統加熱之結果與討論 46 4.1.1 甲烷催化裂解之化學反應機制與建模 46 4.1.2 甲烷催化裂解之化學反應現象 51 4.1.3 溫度與化學反應速率分布 53 4.1.4 流速與反應管徑之影響 58 4.2 微波加熱之結果與討論 66 4.2.1 微波功率對反應系統之影響 66 4.2.2 甲烷流率之影響 74 第五章 結論與未來工作 78 5.1 結論 78 5.1.1 傳統加熱之結論 78 5.1.2 微波加熱之結論 79 5.2 未來工作 80 參考文獻 81 附錄A 90 附錄B 92 自述 94

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