以變壓吸附法純化氣化合成氣經富氧燃燒後高純度二氧化碳之模擬研究

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姓名

陳威宇(Wei-Yu Chen) 查詢紙本館藏

畢業系所

化學工程與材料工程學系

論文名稱

以變壓吸附法純化氣化合成氣經富氧燃燒後高純度二氧化碳之模擬研究
(Simulation of Concentrating High Purity Carbon Dioxide from Syngas after Oxy-fuel Combustion by Pressure Swing Adsorption Process)

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摘要(中)

本研究利用變壓吸附法純化氣化合成氣經富氧燃燒及除水之氣體中二氧化碳，高純度二氧化碳之價值在於其不需經過轉化，可直接作為溶劑與工作/熱傳流體(Working/heat transfer fluid)之用，亦可用於焊接、急速冷凍、設備清洗、醫療、製程反應、晶圓、LED、電子面板等用途，此外，將二氧化碳作為進料，藉由轉化程序，可用以生產化工、生化及電化學產業所需之具有經濟價值之化學品。
合成氣之組成為氫氣、一氧化碳、二氧化碳、甲烷、水及少量的氮氣、氬氣，經過富氧燃燒及除水後，產出約為95%~97.4%二氧化碳濃度氣體及少量氮氣、氬氣，本研究使用UOP 13X沸石作為吸附劑，以Langmuir-Freundlich為模型迴歸吸附劑對各成份氣體的之等溫平衡吸附曲線以取得各項參數，利用理論計算線性驅動力質傳係數用於程序模擬，並與突破曲線實驗、脫附實驗及單塔四步驟程序實驗結果進行驗證，證明程式的可靠度。
最後採用四塔二十四步驟及四塔二十步驟變壓吸附程序進行模擬，藉由探討儲存槽位置、recycle程序之有無及不同的操作變因以尋求最適化操作條件，以無儲存槽附加recycle之四塔二十步驟變壓吸附程序，進料壓力5 atm，塔長105 cm，真空壓力0.238 atm、高壓吸附231秒，同向減壓129秒，抽真空486秒，平衡時間204秒，溫度338.14 K為最佳操作條件，其塔底二氧化碳濃度達99.99994%，回收率9.81%。

摘要(英)

This research studies concentrating carbon dioxide from the syngas of a gasifier after oxy-fuel combustion and dehydration by pressure swing adsorption (PSA) process, so that the concentrated carbon dioxide can be captured and stored to reduce greenhouse gas emission. Zeolite 13X is used in this study. In the beginning of this study, the experimental adsorption isotherm data were regressed to obtain the parameters of Langmuir-Freundlich isotherm equation. Then the k value of linear driving force (LDF) model was calculated by theory and verified by breakthrough curve and desorption experiment. Then we verified the simulation program by comparison with the data of a single-bed four-step process experiment. The agreement is fine. At the end of this study, four-bed twenty-four-step and four-bed twenty-step PSA process for syngas after oxyfuel combustion and dehydration (95% CO2, 5%N2) will be studied to find the optimal operating conditions. The optimal operating conditions are feed pressure 5.00atm, vacuum pressure 0.238atm, adsorption time 231s, cocurrent depressurizaton time 129s, vacuum time 486s, pressurization equilibrium time 204s, temperature 338.14K. The simulation results of optimal operating conditions are 99.99994% purity and 9.81% recovery of carbon dioxide at bottom product of four-bed twenty-step PSA process without tank and with recycle.

關鍵字(中)

★ 變壓吸附
★ 模擬
★ 高純度二氧化碳
★ 富氧燃燒
★ 等溫吸附曲線
★ 突破曲線

關鍵字(英)

★ Pressure swing adsorption
★ Simulation
★ High purity carbon dioxide
★ Oxy-fuel Combustion
★ Isotherm
★ Breakthrough curve

論文目次

摘要 i
ABSTRACT iii
誌謝 v
目錄 vii
圖目錄 x
表目錄 xiv
第一章、緒論 1
第二章、簡介及文獻回顧 5
2-1吸附之簡介 5
2-1-1 吸附基本原理 5
2-1-2 吸附劑及其選擇性 7
2-2 文獻回顧 9
2-2-1 PSA程序之發展與改進 9
2-2-2 理論之回顧 14
2-3研究背景與目的 16
第三章、理論 20
3-1 基本假設 21
3-2 統制方程式 22
3-3 吸附平衡關係式 27
3-3-1 等溫吸附平衡關係式 27
3-3-2 質傳驅動力模式 28
3-3-3 吸附熱關係式 28
3-4 參數推導 29
3-4-1 軸向分散係數 29
3-4-2 熱傳係數 32
3-4-3 線性驅動力質傳係數 35
3-5 邊界條件與流速 39
3-5-1 邊界條件與節點流速 39
3-5-2 閥公式 40
3-6 求解步驟 41
第四章、等溫平衡吸附曲線與吸脫附曲線 44
4-1 吸附平衡(Adsorption Equilibrium) 45
4-1-1 氣體與吸附劑性質 45
4-1-2 等溫平衡吸附曲線(Isotherm) 47
4-2 吸附動力學(Adsorption kinetics) 51
4-2-1 突破曲線模擬驗證 51
4-2-2 脫附實驗模擬驗證 59
第五章、製程描述 63
5-1 單塔四步驟變壓吸附程序 65
5-2 四塔二十四步驟及四塔二十步驟變壓吸附程序 67
5-3 產率與能耗計算 80
第六章、數據分析與結果討論 82
6-1 單塔四步驟變壓吸附法純化合成氣中二氧化碳之驗證 82
6-1-1進料壓力對單塔四步驟PSA製程之驗證 84
6-2 氣化合成氣進料四塔二十四步驟及四塔二十步驟變壓吸附程序之模擬 88
6-2-1 儲存槽及recycle程序對四塔二十四步驟及四塔二十步驟PSA程序之影響及適合純化高純度二氧化碳程序之選擇 91
6-2-2 進料壓力對四塔二十四步驟及四塔二十步驟PSA程序之影響及適合純化高純度二氧化碳程序之選擇 93
6-2-3 進料溫度對四塔二十步驟PSA程序之影響 100
6-2-4 Step 5/10/15/20時間對四塔二十步驟PSA程序之影響 105
6-2-5 塔長對四塔二十步驟PSA程序之影響 109
6-2-6 Step 2/7/12/17時間對四塔二十步驟PSA程序之影響 114
6-2-7 逆向減壓壓力對四塔二十步驟PSA程序之影響 118
6-2-8 最適化結果討論 122
第七章、結論 124
7-1 結論 124
符號說明 127
參考文獻 132
附錄A、流速之估算方法 137

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指導教授

周正堂、楊閎舜(Cheng-Tung Chou Hong-sung Yang)

審核日期

2017-8-22

推文