本論文使用計算流體力學(Computational Fluid Dynamics，CFD) 軟體FLUENT配合一系列之使用者自定函數(User Defined Function, UDF)完成了自甲烷的自熱重組反應(ATR, Autothermal Reforming)生成氫氣之填充床式觸媒反應器(Packed Bed Catalytic Reactor，PBR)之三維模式模擬，模式納入了填充床球型觸媒顆粒反應器中(1)巨相之流力、熱傳與質傳；(2)觸媒顆粒內之流力、熱傳、質傳與化學反應；(3)巨相與觸媒顆粒間之流力、熱傳與質傳。
透過模擬探討了反應器內部之特性分佈，包括壓力、速度、溫度與組成，並探討了參數之影響，包括觸媒球表面處理、雷諾數、孔徑、觸媒球粒徑、不同進氣條件等。針對填充床之摩擦因子以及觸媒顆粒與巨氣相間之熱傳係數與質傳係數，本研究並比較模擬結果與文獻關聯式，結果顯示摩擦因子與Durst等人修正之Ergun方程式較吻合，熱傳係數與質傳係數則分佈零散，並未呈現特別與某一關聯式較吻合之情形。

This thesis uses Computational Fluid Dynamics, combining with a set of User Defined Functions (UDF) to accomplish the simulation studies for the Packed Bed Catalytic Reactor (PBR) for hydrogen generation from steam reforming of methanol.

The model encompasses all important mechanisms for PBR, including (1) the hydraulic, heat and mass transfers of bulk gas; (2) the hydraulic, heat and mass transfers and chemical reaction of catalyst; (3) the hydraulic, heat and mass transfers between bulk gas and catalyst. The simulation is for turbulent flow regime.

The simulation facilitates the discussions on the profiles inside the reactor, including pressure, velocity, temperature and composition. The effects of catalyst particle pore size, catalyst particle diameter, fluid inlet velocity and the location in the reactor are studied. The ways of treating catalyst particle surface friction are investigated too. The friction factor of the bed and the heat and mass transfer coefficients between catalyst particle and bulk gas are compared with the correlations reported in the literature. The friction factor vs. Reynolds number relation is close to the Durst et al. modified Ergun equation, while Nusselt number vs. Reynolds number and Sherwood number vs. Reynolds number relations are scattered distributed and cannot be described well by reported correlations.

致謝……………………………………………………………………………………..i
中文摘要………………………………………………………………………………iii
英文摘要………………………………………………………………………………iv
目錄	v
圖目錄	vii
表目錄	xii
第一章 前言	1
第二章 文獻回顧	3
2.1 填充床式反應器	3
2.2 氫氣生成反應系統	4
第三章 氫氣生成系統	6
3.1化學反應和反應動力	6
第四章 計算流體力學模式之建立	9
4.1系統配置與網格建立	9
4.2 數學模式	13
4.2.1基本統制方程式	13
4.2.2 紊流模式	13
4.2.3 邊界條件	16
4.3 附加程式與設定	18
4.3.1 自訂函數	18
4.3.2 離散方法	21
4.3.3 迭代運算控制參數	22
4.3.4 收斂準則	23
第五章 個案模擬結果	24
5.1 模擬個案總說明	27
5.1.1 個案之設定條件	27
5.1.2反應程度	28
5.1.3有效因子	29
5.1.4 質傳通量	32
5.2 基本個案內部分佈	39
5.2.1 壓力分佈	39
5.2.2 速度分佈	44
5.2.3 溫度分佈	48
5.2.4 組成分佈	53
5.3 個案比較	78
5.3.1 觸媒顆粒表面條件之影響	78
5.3.2 雷諾數之影響	87
5.3.3 孔徑之影響	93
5.3.4 改變觸媒球顆粒粒徑之影響	99
5.3.5 不同進氣條件之影響	106
第六章 輸送係數關聯性之探討	113
6.1 輸送係數之計算	114
6.1.1 流力輸送係數	114
6.1.2熱傳輸送係數	115
6.1.3質傳輸送係數	116
6.2 輸送係數與文獻關聯式之比較	118
6.2.1 流力	118
6.2.2 熱傳	120
6.2.3 質傳	122
6.2.3.1 擴散	123
6.2.3.2 對流及擴散	130
第七章 結論	137
符號說明	141
參考文獻	147
 
圖目錄
圖4-1 填充式反應器觸媒顆粒配置圖，N=4.8637	10
圖4-2 填充式反應器網格圖	11
圖4-3 觸媒顆粒網格繪製示意圖	11
圖5-1 觸媒填充床式反應器之討論截面	26
圖5-2 個案1壓力分佈：S-A、S-B截面	40
圖5-3 個案1壓力分佈：S-C、S-D截面	41
圖5-4 個案1壓力分佈：S-E截面	42
圖5-5 個案1壓力分佈：S-F~S-J截面	43
圖5-6 個案1速度分佈：S-A、S-B截面	45
圖5-7 個案1速度分佈：S-C、S-D截面	46
圖5-8 個案1速度分佈：S-E截面	47
圖5-9 個案1溫度分佈：S-A、S-B截面	49
圖5-10 個案1溫度分佈：S-C、S-D截面	50
圖5-11 個案1溫度分佈：S-E截面	51
圖5-12 個案1溫度分佈：S-F~S-J截面	52
圖5-13 個案1 CH4組成分佈：圖 S-A、S-B截面	54
圖5-14 個案1 CH4組成分佈：S-C、S-D截面	55
圖5-15 個案1 CH4組成分佈：S-E截面	56
圖5-16 個案1 CH4組成分佈：S-F~S-J截面	57
圖5-17 個案1 H2O組成分佈：S-A、S-B截面	58
圖5-18 個案1 H2O組成分佈：S-C、S-D截面	59
圖5-19 個案1 H2O組成分佈：S-E截面	60
圖5-20 個案1 H2O組成分佈：S-F~S-J截面	61
圖5-21 個案1 CO組成分佈：S-A、S-B截面	62
圖5-22 個案1 CO組成分佈：S-C、S-D截面	63
圖5-23 個案1 CO組成分佈：S-E截面	64
圖5-24 個案1 CO組成分佈：S-F~S-J截面	65
圖5-25 個案1 H2組成分佈：S-A、S-B截面	66
圖5-26 個案1 H2組成分佈：S-C、S-D截面	67
圖5-27 個案1 H2組成分佈：S-E截面	68
圖5-28 個案1 H2組成分佈：S-F~S-J截面	69
圖5-29 個案1 CO2組成分佈：S-A、S-B截面	70
圖5-30 個案1 CO2組成分佈：S-C、S-D截面	71
圖5-31 個案1 CO2組成分佈：S-E截面	72
圖5-32 個案1 CO2組成分佈：S-F~S-J截面	73
圖5-33 個案1 O2組成分佈：S-A、S-B截面	74
圖5-34 個案1 O2組成分佈：S-C、S-D截面	75
圖5-35 個案1 O2組成分佈：S-E截面	76
圖5-36 個案1 O2組成分佈：S-F~S-J截面	77
圖5-37 Case 1與Case 8速度分佈比較：S-C截面	82
圖5-38 Case 1與Case 8壓力分佈比較：S-C截面	83
圖5-39 Case 1與Case 8溫度分佈比較：S-C截面	84
圖5-40 Case 1與Case 8 CH4組成分佈比較：S-C截圖	85
圖5-41 Case 1與Case 8 H2組成分佈比較：S-C截圖	86
圖5-42 Case 5與Case 9速度分佈比較：S-C截面	88
圖5-43 Case 5與Case 9溫度分佈比較：S-C截面	89
圖5-44 Case 5與Case9壓力分佈比較：S-C截面	90
圖5-45 Case 5與Case 9 CH4組成分佈比較：S-C截面	91
圖5-46 Case 5與Case 9 H2組成分佈比較：S-C截面	92
圖5-47 Case 1與Case 4速度分佈比較：S-C截面	94
圖5-48 Case 1與Case 4溫度分佈比較：S-C截面	95
圖5-49 Case 1與Case 4壓力分佈比較：S-C截面	96
圖5-50 Case 1與Case 4 CH4組成分佈比較：S-C截面	97
圖5-51 Case 1與Case 4 H2組成分佈比較：S-C截面	98
圖5-52 Case 4與Case 7速度分佈比較：S-C截面	101
圖5-53 Case 4與Case 7壓力分佈比較：S-C截面	102
圖5-54 Case 4與Case 7溫度分佈比較：S-C截面	103
圖5-55 Case 4與Case 7 CH4組成分佈比較：S-C截面	104
圖5-56 Case 4與Case 7 H2組成分佈比較：S-C截面	105
圖5-57 Case 1與Case 6速度分佈比較：S-C截面	108
圖5-58 Case 1與Case 6壓力分佈比較：S-C截面	109
圖5-59 Case 1與Case 6溫度分佈比較：S-C截面	110
圖5-60 Case 1與Case 6 CH4組成分佈比較：S-C截面	111
圖5-61 Case 1與Case 6 H2組成分佈比較：S-C截面	112
圖6-3 質傳係數(Sh_D)之比較,CH4	124
圖6-4 質傳係數(Sh_D)之比較,H2O………………………………………………..125
圖6-5 質傳係數(Sh_D)之比較,CO………………………………….……………..126
圖6-6 質傳係數(Sh_D)之比較,H2…………………...……………………………..127
圖6-7 質傳係數(Sh_D)之比較,CO2………………………………………………..128
圖6-8 質傳係數(Sh_D)之比較,O2…...……………………………………………..129
圖6-9 質傳係數(Sh_T)之比較,CH4………………………………………………..131
圖6-10 質傳係數(Sh_T)之比較,H2O…………..…………………………………..132
圖6-11 質傳係數(Sh_T)之比較,CO………………..……………….……….……..133
圖6-12 質傳係數(Sh_T)之比較,H2………………...………………..……………..134
圖6-13 質傳係數(Sh_T)之比較,CO2………………..……………………………..135
圖6-14 質傳係數(Sh_T)之比較,O2…...………………………..…………………..136
 
表目錄
表3-1 氫氣生成系統反應速率常數之參數值	8
表3-2 氫氣生成系統吸附係數之參數值	8
表4-1 填充式反應器尺寸與網格設定	12
表4-2 邊界條件	16
表4-3 使用之離散方法	21
表4-4 低鬆弛因子設定	22
表4-5 收斂準則	23
表5-1 個案彙整表	25
表5-2 各個案進口物流條件	27
表5-3 反應程度-氫氣生成量 (kmole/s．kgcat)	28
表5-4 有效因子 (R-1)	30
表5-5 有效因子 (R-2)	30
表5-6 有效因子 (R-3)	31
表5-7 有效因子 (R-4)	31
表5-8 CH4質傳量 (kg/s) (自觸媒顆粒至管中流體為正值)	33
表5-9 H2O質傳量 (kg/s) (自觸媒顆粒至管中流體為正值)	34
表5-10 CO質傳量 (kg/s) (自觸媒顆粒至管中流體為正值)	35
表5-11 H2質傳量 (kg/s) (自觸媒顆粒至管中流體為正值)	36
表5-12 CO2質傳量 (kg/s) (自觸媒顆粒至管中流體為正值)	37
表5-13 O2質傳量 (kg/s) (自觸媒顆粒至管中流體為正值)	38
表5-14 改變觸媒顆粒表面條件對反應程度-氫氣生成量之影響	78
表5-15 改變觸媒顆粒表面條件對CH4 (kg/s)質傳量之影響	79
表5-16 改變觸媒顆粒表面條件對H2O (kg/s)質傳量之影響	79
表5-17 改變觸媒顆粒表面條件對CO (kg/s)質傳量之影響	79
表5-18 改變觸媒顆粒表面條件對H2 (kg/s)質傳量之影響	80
表5-19 改變觸媒顆粒表面條件對CO2 (kg/s)質傳量之影響	80
表5-20 改變觸媒顆粒表面條件對O2 (kg/s)質傳量之影響	80
表5-21 改變雷諾數對反應程度-氫氣生成量之影響	87
表5-22 改變孔徑對反應程度-氫氣生成量之影響	93
表5-23 改變觸媒球粒徑對反應程度-氫氣生成量之影響 (kmole/s．kgcat)	100
表5-24 有效因子 (R-1)	100
表5-25 有效因子 (R-2)	100
表5-26 有效因子 (R-3)	100
表5-27 有效因子 (R-4)	100
表5-28 不同進氣條件對反應程度-氫氣生成量之影響 (kmole/s．kgcat)	107
表5-29 有效因子 (R-1)	107
表5-30 有效因子 (R-2)	107
表5-31 有效因子 (R-3)	107
表5-32 有效因子 (R-4)	107

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