碳排放之管制將有大量來自電廠與製程之二氧化碳捕獲，利用二氧化碳生產的甲醇可以做為燃料或化學品，是最可行的二氧化碳再利用方式之一。乙烯/丙烯是石化工業上游大宗原料，可以透過甲醇製造烯烴(MTO, Methanol to Olefins)技術生產。本論文針對工業級甲醇轉烯烴製程進行完整流程設計，包括反應段、分離段與冷凍循環，並針對最耗能的產物分離與回收段程序進行優化設計，採用蒸餾塔能耗目標分析改善蒸餾序列各蒸餾塔之設計，並納入冷箱以改善最低溫段的分離性能與能效。
甲醇製烯烴製程採用UOP/Hydro反應器性能，同時生產36萬噸/年乙烯與36萬噸/年丙烯。相較於基本個案設計，優化設計之可用能損失降低了40%，乙烯損失率降低了36%。優化設計之IRR為30.2%且甲醇價格對經濟效益影響重大。甲醇轉烯烴程序之單位產品能耗與二氧化碳排放分別為1.9 GJ/MT乙烯與0.3 MT CO2/MT olefins，均低於傳統蒸氣裂解製程，若涵蓋前端利用二氧化碳之甲烷產甲醇製程，則可獲得淨減碳的效益，達-0.4 MT CO2/MT olefins。

Carbon emission control will generate significant amount of carbon dioxide from the carbon capture facilities of power plants and various industries. Generation of methanol as fuel or chemical is one of the most feasible way of carbon dioxide utilization. Furthermore, ethylene and propylene, which are the most important commodity raw materials of petrochemical industry, can be produced from methanol via the methanol-to-olefins (MTO) technology. This thesis presents the overall process design, including reaction and separation sections as well as refrigeration cycles, of an industrial-scale MTO process. Optimal design focuses on the product separation and recovery section, which is the most energy consuming part of the process. Column targeting analysis is employed to improve distillation column design and a cold-box is added to improve the separation performance and energy utilization of the lowest-temperature part of the process.
The MTO process is based on the reactor performance of UOP/Hydro technology and produces polymer-grade ethylene and propylene with a capacity of 360 kt/y each. Compared to the base design, the optimal design reduces the exergy loss by 40%, the ethylene loss rate is reduced by 36%. The IRR of the optimal design is 30.2% and is highly dependent on the methanol price. The optimal MTO process is superior to the conventional ethane and naphtha steam cracking in energy consumption and carbon dioxide emission and the results are 1.9 GJ/MT ethylene and 0.3 MT CO2/MT olefins, respectively. The combination of the MTO process and its feedstock production process, i.e. the methanol process from methane reforming with utilization of carbon dioxide, generates a carbon reduction effect of 0.4 MT CO2/MT olefins.

目錄
中英文摘要	I
目錄	III
表目錄	VII
圖目錄	XII
第一章 緒論	1
1.1 前言	1
1.1.1 甲醇製程	3
1.1.2	甲醇製乙烯與丙烯製程	6
1.2 研究目的、範疇與方法	9
1.3 論文組織架構	11
第二章 文獻整理	12
第三章 基本個案設計	18
3.1設計規範	18
3.2方塊流程	20
3.3程序流程	22
3.3.1 甲烷多元重組製甲醇之程序流程	22
3.3.2 甲烷轉烯烴之基本個案設計程序流程	25
3.4 反應器設計	45
3.5 蒸餾序列設計	47
3.6 蒸餾塔設計	50
3.7冷凍系統設計	53
第四章 甲烷轉烯烴程序產物分離與回收段之優化設計	54
4.1 蒸餾塔能耗目標分析	54
4.2甲烷轉烯烴程序產品分離與回收段各塔之優化設計	65
4.2.1冷凝液分離塔	65
4.2.2 去甲烷塔	66
4.2.3去乙烷塔	67
4.2.4乙烯分離塔	69
4.2.5去丙烷塔	71
4.2.6丙烯分離塔	72
4.3 冷箱設計	73
4.4 基本個案設計與優化設計之比較	80
4.5 優化設計流程說明	85
4.5.1 產物分離與回收段	86
4.5.2 冷箱流程	93
4.5.3 冷凍系統	97
第五章 能源整合及可用能分析	108
5.1甲烷轉烯烴之熱整合	108
5.2 可用能分析	115
第六章 設備規格與公用設施	118
6.1 設備規格	118
6.2 公用設施	124
第七章 經濟效益、能耗與減碳分析	128
7.1 設備成本	128
7.1.1 反應器	129
7.1.2 蒸餾塔	129
7.1.3 熱交換器	131
7.1.4 壓力控制單元	135
7.1.5 總設備成本	136
7.2 總投資成本	137
7.3 製造成本	138
7.3.1 直接製造成本	138
7.3.2 固定製造成本與一般費用	142
7.3.3 總製造成本	143
7.4 經濟效益分析	144
7.4.1 現金流分析	144
7.4.2 淨現值分析	146
7.4.3 內部報酬率與投資報酬率	147
7.5 能耗分析	148
7.6 碳排放分析	151
7.7 經濟分析總結	154
第八章 結論	158
符號說明	160
參考文獻	162

 
表目錄
表3.1 產品設計規格表	19
表3.2 甲烷轉烯烴反應與調理段物流資料	28
表3.2 甲烷轉烯烴反應與調理段物流資料(續一)	29
表3.3 甲烷轉烯烴製程基本個案設計產物分離與回收段物流資料	34
表3.3 甲烷轉烯烴製程基本個案設計產物分離與回收段物流資料(續一)	35
表3.3 甲烷轉烯烴製程基本個案設計產物分離與回收段物流資料(續二)	36
表3.4 甲烷轉烯烴製程基本個案設計冷凍循環物流資料	40
表3.4 甲烷轉烯烴製程基本個案設計冷凍循環物流資料(續一)	41
表3.4 甲烷轉烯烴製程基本個案設計冷凍循環物流資料(續二)	42
表3.4 甲烷轉烯烴製程基本個案設計冷凍循環物流資料(續三)	43
表3.4 甲烷轉烯烴製程基本個案設計冷凍循環物流資料(續四)	44
表3.5 UOP/Hydro MTO反應器質量產率 (Hannula, 2015)	46
表3.6 甲烷轉烯烴製程產物分離與回收段進料之組成與相對揮發度	49
表3.7 甲烷轉烯烴基本個案設計之蒸餾塔設計條件	50
表3.8 傳統蒸氣裂解與甲烷轉烯烴製程分離程序之蒸餾塔塔壓比較	52
表3.9 甲烷轉烯烴基本個案設計之冷媒等級與熱負荷量需求	53
表4.1 MTO程序各塔之進料組成條件與輕重關鍵成分(灰底與粗體分別為輕重關鍵成分)	61
表4.2 冷箱進料條件比較	75
表4.3 冷箱各相分離器之操作條件	78
表4.4 基本設計與優化設計之C1分離段能耗比較	78
表4.5 甲烷轉烯烴製程反應段設計條件	80
表4.6 產物分離與回收段設計比較	82
表4.7 冷凍系統設計之比較	83
表4.8 優化設計之影響	83
表4.9 基本個案設計與優化設計作功單元能耗比較(kW)	84
表4.10 甲烷轉烯烴製程優化設計之產物分離與回收段物流資料	89
表4.10 甲烷轉烯烴製程優化設計之產物分離與回收段物流資料(續一)	90
表4.10 甲烷轉烯烴製程優化設計之產物分離與回收段物流資料(續二)	91
表4.10 甲烷轉烯烴製程優化設計之產物分離與回收段物流資料(續三)	92
表4.11冷箱設計物流資料	94
表4.11冷箱設計物流資料(續一)	95
表4.11冷箱設計物流資料(續二)	96
表4.12甲烷轉烯烴製程優化設計之冷凍循環物流資料	100
表4.12甲烷轉烯烴製程優化設計之冷凍循環物流資料(續一)	101
表4.12甲烷轉烯烴製程優化設計之冷凍循環物流資料(續二)	102
表4.12甲烷轉烯烴製程優化設計之冷凍循環物流資料(續三)	103
表4.12甲烷轉烯烴製程優化設計之冷凍循環物流資料(續四)	104
表4.12甲烷轉烯烴製程優化設計之冷凍循環物流資料(續五)	105
表4.12甲烷轉烯烴製程優化設計之冷凍循環物流資料(續六)	106
表4.12甲烷轉烯烴製程優化設計之冷凍循環物流資料(續七)	107
表5.1 優化設計之熱交換物流資料	110
表5.2 基本設計與優化設計之可用能損失(MJ/s)	116
表6.1 甲烷轉烯烴製程優化設計之蒸餾塔設計結果	119
表6.1 甲烷轉烯烴製程優化設計之蒸餾塔設計結果(續一)	120
表6.1 甲烷轉烯烴製程優化設計之蒸餾塔設計結果(續二)	120
表6.2 甲烷轉烯烴製程優化設計之熱交換器設備規格	121
表6.2 甲烷轉烯烴製程優化設計之熱交換器設備規格(續一)	122
表6.2 甲烷轉烯烴製程優化設計之熱交換器設備規格(續二)	123
表6.3 甲烷轉烯烴製程優化設計之公用設施清單	125
表6.3 甲烷轉烯烴製程優化設計之公用設施清單(續一)	126
表6.3 甲烷轉烯烴製程優化設計之公用設施清單(續二)	127
表7.1 蒸餾塔之設備成本	130
表7.2 蒸餾塔之塔板成本	130
表7.3 蒸餾塔裸模成本	131
表7.4 優化設計熱整合之熱交換器成本	132
表7.5 優化設計冷箱之熱交換器成本	134
表7.6 幫浦之設備成本	135
表7.7 壓縮機之設備成本	135
表7.8 甲烷轉烯烴優化設計設備成本	136
表7.9 甲烷轉烯烴優化設計總投資成本($)	137
表7.10 直接製造成本項目	138
表7.11 甲烷轉烯烴優化設計之直接製造成本(MM$/year)	139
表7.12 公用設施單價	139
表7.13 甲烷轉烯烴優化設計之公用設施成本	140
表7.14原料單價及成本	141
表7.15 固定成本之項目	142
表7.16 一般製造之項目	142
表7.17 甲烷轉烯烴優化設計之總製造成本彙整	143
表7.18 現金流分析方式	145
表7.19 甲烷轉烯烴優化設計之現金流	145
表7.20 甲烷轉烯烴優化設計之收入	146
表7.21 耗功單元之能耗(kW)	149
表7.22 烯烴生產後段分離程序進料比較(mass%)	150
表7.23 烯烴生產程序之能耗比較(GJ/MT乙烯)	151
表7.24 不同烯烴製造路徑之二氧化碳排放比較	153
表7.25 甲烷轉烯烴優化設計各類成本及經濟分析總結	154
表7.26不同甲醇價格之各類經濟指標比較	157
 
圖目錄
圖1.1 CO2之捕獲與再利用機會(NETL)	2
圖1.2 各式原料生產合成氣、甲醇、各種化學品及燃料之路徑	2
圖1.3不同類型反應與二氧化碳添加方法之甲醇生產程序	6
圖1.4 UOP/Norsk Hydro甲醇轉烯烴技術	6
圖1.5 Lurgi MTP技術	7
圖1.6 全球甲醇應用領域及使用量(Alvarado, 2016)	7
圖1.7 UOP MTO/Total OCP process流程	8
圖1.8 Lurgi MTP流程	9
圖3.1 甲烷-甲醇-烯烴整合程序方塊流程	21
圖3.2 甲烷多元重組製甲醇之程序流程	24
圖3.3 甲烷轉烯烴程序之反應與調理段流程	27
圖3.4 甲烷轉烯烴程序之基本個案設計產物分離與回收段流程	33
圖3.5 甲烷轉烯烴程序之乙烯冷凍循環	38
圖3.6 甲烷轉烯烴程序之丙烯冷凍循環	39
圖3.7 甲醇轉烯烴流體化床反應器	45
圖3.8 甲烷轉烯烴製程產物分離與回收段之蒸餾序列	49
圖4.1 雙成分最小熱力蒸餾塔(MTC)	55
圖4.2 多成分最小熱力蒸餾塔	55
圖4.3 實務接近最小熱力條件(PNMTC)	56
圖4.4 簡單蒸餾塔的CGCC圖	56
圖4.5 由CGCC呈現塔之各種改善之能源利用目標	57
圖4.6 利用各板之模擬組成求解CGCC	58
圖4.7 每一板的焓差額決定	59
圖4.8 以每板的焓差額建立CGCC圖	59
圖4.9 CGCC圖與CCC圖	60
圖4.10 Column analysis選項	62
圖4.11 關鍵成分選取模式頁面	62
圖4.12 多種關鍵成分選取	63
圖4.13 Column analysis 分析結果展示與繪製CGCC	63
圖4.14 調整回流比之影響	64
圖4.15 冷凝液分離塔調整設計前之CGCC	65
圖4.16 冷凝液分離塔調整設計後之CGCC	66
圖4.17 冷凝液分離塔調整設計前後之CCC	66
圖4.18 去甲烷塔之CGCC	67
圖4.19 去甲烷塔之CCC	67
圖4.20 去乙烷塔調整設計前之CGCC	68
圖4.21 去乙烷塔調整設計後之CGCC	68
圖4.22 去乙烷塔調整設計前後之CCC	69
圖4.23 乙烯分離塔調整設計前之CGCC	70
圖4.24 乙烯分離塔調整設計後之CGCC	70
圖4.25 乙烯分離塔之CCC	70
圖4.26 去丙烷塔之CGCC	71
圖4.27 去丙烷塔之CCC	71
圖4.28 丙烯分離塔之CGCC	72
圖4.29 丙烯分離塔之CCC	72
圖4.30 典型的乙烯製程冷箱系統(Zhang et al., 2010)	74
圖4.31 甲烷轉烯烴程序之冷箱系統	76
圖4.32 冷箱多物流熱交換器CB1~CB7之冷熱複合曲線	79
圖4.33 基本個案設計與優化設計作功單元能耗佔比	85
圖4.34 基本個案設計與優化設計作功單元能耗佔比	85
圖4.35甲烷轉烯烴製程優化設計之產品分離與回收段流程	88
圖4.36 甲烷轉烯烴製程優化設計之乙烯冷凍循環流程	98
圖4.37 甲烷轉烯烴製程優化設計之丙烯冷凍循環流程	99
圖5.1 優化設計冷熱複合曲線(ΔTmin=10℃)	111
圖5.2優化設計之總複合曲線(ΔTmin=10℃)	112
圖5.3 甲烷轉烯烴製程優化設計之熱交換網路(常溫以上, ∆Tmin = 10℃)	113
圖5.4 甲烷轉烯烴製程優化設計熱交換網路(常溫以下, ∆Tmin = 2℃)	114
圖5.5 基本個案設計各類設備之可用能損失	116
圖5.6 優化設計各類設備之可用能損失	117
圖7.1 MHeatX熱交換器內部分區分析結果示例	133
圖7.2 甲烷轉烯烴優化設計各類設備成本佔比	136
圖7.3 甲烷轉烯烴優化設計公用設施成本佔比	140
圖7.4 不同甲醇價格($/MT)之甲烷轉烯烴製程NPV比較	156
圖7.5 不同甲醇價格($/MT)之甲烷轉烯烴製程IRR比較	156
圖7.6 不同甲醇價格($/MT)之甲烷轉烯烴製程ROI比較	157

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