本論文中以Aspen Plus 模擬軟體建立水轉移反應系統數學模式，並與文獻實驗數據確認其準確度。水轉移反應器結構分成單一及兩顆水轉移反應系統來探討。根據水轉移反應模式，最適化問題為改變反應器進口溫度、進料組成及一氧化碳轉化率之最小水轉移反應器體積，燃料處理系統出口氫氣流量需要滿足2.2 kW之質子交換膜燃料電池使用，一氧化碳濃度限制在20 ppm。結果顯示當一氧化碳轉化率超過平衡轉化率時，含有熱交換器之兩顆水轉移反應系統之反應系統體積會大幅減少。從建立出來之設計通則可以快速決定水轉移反應系統流程。由靈敏度分析可以得到水轉移反應系統控制架構。操作度分析結果顯示當氫氣流量改變，單一水轉移反應系統操作範圍會比兩顆水轉移反應系統來的大，兩顆水轉移反應系統之操作度因為進口一氧化碳濃度增加而減少。

In this work, Aspen plus simulation software were used to develop a model to describe  water gas shift (WGS) reactor systems which validated with experimental data. The WGS reactor structures, single and two, were investigated. Based on the WGS reactor systems model, optimization problem was formulated and performed to minimize the reactor volume by varying reactor inlet temperatures and feed compositions and CO conversion while maintaining the hydrogen flow rate (2.2 kW PEMFC used) and CO concentration constraint 20 ppm. The results show that two WGS reactors in series systems with intercoolers can largely reduce the reaction volume when CO conversion exceeded equilibrium conversion.Then, design heuristic was built to provide a quick determination of WGS reactor system flowsheet. After sensitivity analysis was made, control structures are explored here.The result shows single WGS reactor system has larger operability range than two WGS reactors in series during hydrogen throughput change. Operability range of two WGS reactors in series systems was reduced by an increasing inlet CO composition.

目錄
中文摘要	I
英文摘要	II
目錄	III
圖目錄	VII
表目錄	XII
第一章、緒論	1
1.1.	前言	1
1.2.	文獻回顧	5
1.3.	研究動機	9
1.4.	論文組織	9
第二章、從碳氫化合物之蒸氣重組產生氫氣	11
2.1系統描述	11
2.2碳氫化合物的來源	13
2.2.1烷類蒸氣重組	13
2.2.2醇類蒸氣重組	20
2.2.3高碳數碳氫化合物	26
2.3水轉移反應	31
2.3.1水轉移反應器進料組成	31
2.3.2水轉移反應平衡常數	32
2.3.3水轉移反應平衡轉化率	33
2.4水轉移反應觸媒與動力學	39
2.5總結	45
第三章、絕熱水轉移反應系統之體積最小化設計	46
3.1水轉移反應系統之模式建立與模式驗證	46
3.1.1 模式假設	47
3.1.2 模式	47
3.1.3 模擬結果與模式驗証	51
3.2單一與串聯水轉移反應系統之設計最適化	53
3.2.1目標函數與最適化變數	55
3.2.2單一水轉移反應系統之最適化設計	56
3.2.3串聯水轉移反應系統之最適化設計	57
3.3水轉移反應系統設計選擇	64
3.3.1產品規格	64
3.3.2不同轉化率下水轉移反應器選擇	65
3.3.3不同進料組成下水轉移反應系統選擇	71
3.3.3.1 一氧化碳莫耳分率(yCO)改變	71
3.3.3.2 λ值改變	75
3.3.3.3水之莫耳分率(yH2O)改變	79
3.4水轉移反應系統設備成本分析	81
3.5單位水轉移反應系統體積之一氧化碳轉化效能(X.E.)	85
3.6結果與討論	89
3.6.1水轉移反應系統之設計經驗法則	89
3.6.2水轉移反應系統選擇區塊	94
3.7總結	97
第四章、控制架構設計及操作度	98
4.1控制目標	99
4.2水轉移反應系統靈敏度分析	99
4.2.1水轉移反應系統操作溫度之影響	100
4.2.2水轉移反應系統進料水量之影響	107
4.3水轉移反應系統控制架構設計	111
4.4 水轉移反應系統操作度分析	113
4.4.1單一水轉移反應系統操作度分析114
4.4.2串聯水轉移反應系統操作度分析121
4.4.3結果與討論	127
4.5總結	134
五、結論	136
符號說明	137
參考文獻	141
附錄	153
圖目錄
圖2-1、燃料處理器程序流程圖	12
圖2-2、水轉移反應平衡常數對溫度關係圖	33
圖2-3、水轉移反應進料組成無因次與轉化率表示圖	33
圖2-4、碳氫化合物水轉移反應之平衡轉化率對不同碳氫化合物進料組成關係圖36
圖3-1、高溫絶熱水轉移反應器串聯系統流程圖	47
圖3-2、各成分莫耳流率及溫度對水轉移反應器體積關係圖	52
圖3-3、(a) 單一, (b) 串聯高溫絶熱水轉移反應系統流程圖	54
圖3-4、(a) 單一水轉移反應系統, (b) 串聯水轉移反應系統體積最適化物流資料表	58
圖3-5、體積最適化水轉移反應系統溫度分布對一氧化碳轉化率關係圖	61
圖3-6、最適化體積之水轉移反應系統各成分濃度、反應速率以及溫度對反應器體積關係圖	63
圖3-7、yCO=3.5 mol%，yH2O=40.8 mol%及λ=5.3，單一與串聯水轉移反應系統之進出口溫度、總體積變化差異、總流量、出口氫氣量及反應器體積佔有率對一氧化碳轉化率關係圖	70
圖3-8、yCO=10.6 mol%，yH2O=40.8 mol%及λ=5.3，單一與串聯水轉移反應系統之進出口溫度、總體積變化差異、總流量、出口氫氣量及反應器體積佔有率對一氧化碳轉化率關係圖	73
圖3-9、yCO=2.6 mol%，yH2O=40.8 mol%及λ=5.3，單一與串聯水轉移反應系統之進出口溫度、總體積變化差異、總流量、出口氫氣量及反應器體積佔有率對一氧化碳轉化率關係圖	74
圖3-10、yCO=2.6 mol%，yH2O=40.8 mol%及λ=2.9，單一與串聯水轉移反應系統之進出口溫度、總體積變化差異、總流量、出口氫氣量及反應器體積佔有率對一氧化碳轉化率關係圖	77
圖3-11、yCO=2.6 mol%，yH2O=40.8 mol%及λ=1.1，單一與串聯水轉移反應系統之進出口溫度、總體積變化差異、總流量、出口氫氣量及反應器體積佔有率對一氧化碳轉化率關係圖	78
圖3-12、yCO=2.6 mol%，yH2O=33.5 mol%及λ=2.9，單一與串聯水轉移反應系統之進出口溫度、總體積變化差異、總流量、出口氫氣量及反應器體積佔有率對一氧化碳轉化率關係圖	80
圖3-13、不同進料組成下，水轉移反應系統之反應器設備成本對一氧化碳轉化率關係圖	83
圖3-14、不同進料組成下，水轉移反應系統設備成本對一氧化碳轉化率關係圖	84
圖3-15、不同進料組成之下，單位水轉反應系統體積之一氧化碳轉化效能對一氧化碳轉化率關係圖	86
圖3-16、單位水轉反應器體積之一氧化碳轉化效能對一氧化碳轉化率關係圖	88
圖3-17、不同進料組成水轉移反應系統總體積變化對一氧化碳轉化率關係圖	90
圖3-18、水轉移反應系統選擇對一氧化碳轉化率關係圖	93
圖3-19、(a) 不同水轉移觸媒, (b) 改變yCO, (c) 改變λ值 (d) 改變yH2O溫度對一氧化碳轉化率關係圖	96
圖4-1、用電負荷量及氫氣需求量示意圖	99
圖4-2、單一水轉移反應系統改變進口溫度對於反應器出口溫度、水轉移反應速率、出口組成關係圖	102
圖4-3、串聯水轉移反應系統改變第一顆反應器進口溫度對反應器出口溫度、水轉移反應速率、出口組成關係圖	105
圖4-4、串聯水轉移反應系統改變第二顆反應器進口溫度對反應器出口溫度、水轉移反應速率、出口組成關係圖	106
圖4-5、單一水轉移反應系統改變進料添加水量對反應器出口溫度、水轉移反應速率、出口組成關係圖	108
圖4-6、串聯水轉移反應系統改變進料添加水量對反應器出口溫度、水轉移反應速率、出口組成關係圖	110
圖4.7、(a) 單一, (b) 串聯水轉移反應系統濃度控制結構圖	112
圖4.8、(a) 單一, (b) 串聯水轉移反應系統存量控制結構圖	113
圖4-9、單一水轉移反應系統(a) 操作度分布, (b) A1(ΔFTot=100 %), (c) B1(ΔFTot=55.3%), (d) C1(ΔFTot=30 %)溫度分布圖	116
圖4-10、單一水轉移反應系統(a) 操作度分布, (b) A2(ΔFTot=100 %), (c) B2(ΔFTot=61.3 %), (d) C2(ΔFTot=30 %)溫度分布圖	118
圖4-11、單一水轉移反應系統(a) 操作度分布, (b) A3(ΔFTot=100 %), (c) B3(ΔFTot=50 %), (d) C3(ΔFTot=99.9 %)溫度分布圖	120
圖4-12、串聯水轉移反應系統(a) 操作度分布, (b) A1(ΔFTot=100 %), (c) B1(ΔFTot=42.4 %), (d) C1(ΔFTot=30 %)溫度分布圖	122
圖4-13、串聯水轉移反應系統(a) 操作度分布, (b) A1(FTot=100 %), (c) B2(ΔFTot=66.2 %), (d) C2(ΔFTot=30 %)溫度分布圖	124
圖4-14、串聯水轉移反應系統(a) 操作度分布, (b) A3(ΔFTot=100 %), (c) B3(ΔFTot=50 %), (d) C3(ΔFTot=99.9 %)溫度分布圖	126
圖4-15、不同進料組成之水轉移反應系統操作度對一氧化碳轉化率關係圖	128
圖4-16、XCO=80.6 %，yCO=3.5 mol%，yH2O=40.8 mol%及λ值為5.3，ΔFTot=49.5%串聯水轉移系統溫度分佈圖	130
圖4-17、XCO=80%，yCO=10.6 mol%，yH2O=40.8 mol%及λ值為5.3，ΔFTot=86.4 %串聯水轉移系統溫度分佈圖	132
圖4-18、不同進料一氧化碳濃度下，串聯水轉移反應系統之(a) 總流量需求, (b) 一氧化碳反應量, (c) 操作度, (d) XCO=80 %，達操作溫度上限之溫度分布圖133
表目錄
表1-1、低碳數烷類碳氫化合物水轉移反應系統結構整理表	7
表1-2、醇類及高碳數碳氫化合物水轉移反應系統結構整理表	8
表2-1、碳氫化合物蒸氣重組反應途徑整理表	15
表2-2、甲烷蒸氣重組文獻整理表	16
表2-3、乙烷蒸氣重組之文獻整理表	19
表2-4、甲醇蒸氣重組文獻整表	21
表2-5、乙醇蒸氣重組之文獻整理表	24
表2-6、乙醇蒸氣重組之文獻整理表(續)	25
表2-7、液化石油氣蒸氣重組文獻整理表	28
表2-8、柴油蒸氣重組文獻整理表	30
表2-9、烷類碳氫化合物進料組成與水轉移反應之平衡轉化率整理表	37
表2-10、醇類及高碳數碳氫化合物進料組成與水轉移反應之平衡轉化率整理表	38
表2.11、高溫水轉移觸媒整理表	40
表2.12、高溫水轉移觸媒整理表(續)	41
表2-13、低溫水轉移觸媒整理表	43
表2-14、低溫水轉移觸媒整理表(續)	44
表3-1、蒸氣重組系統之各個反應器進出口端物流組成與溫度數據	49
表3-2、水轉移反應器尺寸及觸媒用量	50
表3-3、最適化水轉移反應系統總體積與操作溫度比較表	59

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