本研究採用COMSOL Multiphysics 5.5 套裝軟體，利用數值模擬探討鈀膜助效式甲烷蒸汽重組反應器在不同參數條件下對於反應器的效率影響。本研究使用Ni-Pt/CeZnLa觸媒，觸媒添加量為0.232kg，探討反應器內管(滲透端)半徑為6.25mm、外管(反應端)半徑為20.625mm，整體觸媒床長度為400mm，前後各有50mm的未反應區，總長為500mm。入口甲烷流率為0.208~1.66×10^-5(m^3/s)、壁溫為673~873K、入口溫度為673~773K、水碳比為2~4、掃氣量為1.6×10^-5~ 2.56×10^-4 (m^3/s)。
透過數值模擬結果，甲烷流率的增加導致觸媒床入口冷區擴大，降低重組效率，流率的增加亦降低進料停留在觸媒床的反應時間，並影響氫氣擴散到薄膜的效率，降低整體甲烷轉化率與氫氣回收率(99.5→45.3%、95.2→47%)。壁溫的提升將整體反應器的甲烷轉化率提高(40.4→99.2%)，並增加薄膜的穿透率(3.6×10^-7→3.8×10^-7kgm^-2^s-1)，但穿透率的提升幅度不如重組速率的提升幅度(0.017→0.034molm^-3^s-1)，使氫氣會累積在反應器壁面，反應器分壓上升，滲透性透過穿透率上升與反應端分壓的上升而快速上升。進料溫度上升影響不如壁溫，但對整體反應器達到均溫的效果，在反應端薄膜側的重組速率提高，使氫氣產生後能夠快速地滲透到薄膜側，提高滲透效應，甲烷轉化率與氫氣回收率上升(77.9→92.6%、75.8→92.3%)。水碳比的上升(2→4)將降低反應端氫氣分壓，降低甲烷轉化率(87.3→81.6%)，並提高成本，因此水碳比建議為化學莫耳當量(甲烷為2)。掃氣量的上升[1.6×10^-5~ 2.56×10^-4 (m^3/s)]能夠提高甲烷轉化率與氫氣回收率(58.1→97.8%、58.2%→97.5%)，但掃氣較高時提升較不明顯。甲烷轉化率的提升與掃氣倍率呈線性關係，直到甲烷轉化率達到85%以上，此後的掃氣量提升的甲烷轉化率逐漸降低。
為了使薄膜滲透效應明顯，在整體反應器的壁溫應達到773K以上以維持足夠的氫氣產出，透過適當的提高入口溫度，能夠將整體重組效率的高峰由壁面變成薄膜側，並將整體反應區的冷區向觸媒床尾端移動，增加觸媒床入口附近的效率。

In this study, the COMSOL Multiphysics 5.5 software package was used to investigate the effect of the palladium membrane-assisted methane steam reforming reactor on the efficiency of the reactor under different parameter conditions by numerical simulation. In this study, Ni-Pt/CeZnLa catalyst has been used. The catalyst addition amount was 0.232kg. The radius of the inner tube (permeate side) of the reactor is 6.25mm, the radius of the outer tube (reactant side) is 20.625mm, and the overall catalyst bed length was 400mm, there are 50mm unreacted areas at the front and back, and the total length is 500mm. The inlet methane flow rate is 0.208~1.66×10^-5(m^3/s), the wall temperature is 673~873K, the inlet temperature is 673~773K, the water to carbon ratio is 2~4, sweep flow rate is 1.6×10^-5~ 2.56×10^-4 (m^3/s).
Through numerical simulation results, the increase in methane flow rate leads to the expansion of the cold zone at the inlet of the catalyst bed, which reduces the reforming efficiency. The increase in flow rate also reduces the reaction time of the feed staying in the catalyst bed, and affects the efficiency of hydrogen diffuse to the membrane. The overall methane conversion and hydrogen recovery decrease(99.5→45.3%、95.2→47%). The increase in wall temperature increasing the methane conversion of the overall reactor(40.4→99.2%) and increasing the permeate rate of the membrane(3.6×10^-7→3.8×10^-7kgm^-2^s-1), but the increase in permeate rate is not as good as reforming rate(0.017→0.034molm^-3^s-1), so that hydrogen will accumulate on the wall of the reactor and the partial pressure of the reactor will increase. The permeance rises rapidly through the increase in the permeate rate and the increase in the partial pressure of the reaction side. The increase in feed temperature is not as good as the wall temperature, but it makes the temperature of the entire reactor uniform . The reforming rate at the membrane side of the reaction side is improved, so that the hydrogen can quickly permeate to the membrane side after generation, and the permeation effect is improved. Methane conversion and hydrogen recovery increase(77.9→92.6%、75.8→92.3%). An increase in the water to carbon ratio(2→4) will reduce the hydrogen partial pressure at the reaction side, reduce the methane conversion (87.3→81.6%), and increase the cost. Therefore, the water to carbon ratio is recommended to be chemical molar equivalent (methane is 2). The increase of sweep flow rate[1.6×10^-5~ 2.56×10^-4 (m^3/s)]can increase the methane conversion and the hydrogen recovery rate(58.1→97.8%、58.2%→97.5%) , but the improvement is not obvious when the sweep flow rate is higher. The increase of the methane conversion has a linear relationship with the sweep flow rate magnification until the methane conversion reaches over 85%, after which the methane conversion of the sweep flow rate increase gradually decreases.
In order to make the membrane permeation effect obvious, the wall temperature of the overall reactor should be above 773K to maintain sufficient hydrogen production. By appropriately increasing the inlet temperature, the peak of the overall reforming efficiency can be changed from the wall surface to membrane side, making the cold zone move form the inlet of the catalyst bed to the end of the catalyst bed to increase the efficiency near the entrance of the catalyst bed.

摘要 i
Abstract ii
目錄 iv
圖目錄 vii
表目錄 xi
符號說明 xii
第一章 緒論 1
1.1 前言 1
1.2 燃料電池 5
1.2.1 燃料電池原理 5
1.2.2 燃料電池元件 6
1.2.3 市面燃料電池 8
1.3 化石燃料重組產氫 11
1.3.1 蒸汽重組(Steam reforming、SR) 11
1.3.2部分氧化(Partial oxidation , POX) 15
1.3.3自熱重組(Autothermal reforming , ATR) 16
1.3.4煤炭氣化 (Coal Gasification , CG) 17
1.3.5電漿重組 (Plasma Reformer , PR) 19
1.4 研究目的 20
第二章 文獻回顧 21
2.1 薄膜材料 22
2.2 氣體滲透程序 24
2.3 薄膜滲透性 26
2.4 薄膜相關文獻 27
第三章 數值方法 31
3.1 反應器 31
3.2 假設 33
3.3 統御方程式(Continuity equation) 34
3.3.1 質量守恆方程式(穩態) (Continuity equation) 34
3.3.2 動量方程式(Momentum equation) 34
3.3.3 能量方程式(Energy equation) 34
3.3.4 成分方程式(Species equation) 35
3.4 甲烷蒸汽重組反應方程式 36
3.5 初始與邊界條件 39
3.5.1 邊界條件(Boundary condition) 39
3.5.2 初始條件(Initial condition) 40
3.6 參數選擇 41
3.7 網格測試 42
3.8 模型驗證 43
第四章 結果與討論 45
4.1 反應器內部反應 46
4.2 甲烷入口流率影響 54
4.3 反應端壁溫影響 67
4.4 進料溫度影響 81
4.5 水碳比影響 88
4.6 掃氣量影響 94
第五章 結論與未來建議 102
5.1 結論 102
5.2 未來建議 104
參考文獻 105

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