利用吸附程序於較小型發電廠煙道氣進氣量下捕獲二氧化碳之模擬

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王彥翔(Yen-hsiang Wang) 查詢紙本館藏

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化學工程與材料工程學系

論文名稱

利用吸附程序於較小型發電廠煙道氣進氣量下捕獲二氧化碳之模擬
(Simulation of Carbon Dioxide Capture from Small Power Plant Flue Gas by Adsorption)

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摘要(中)

本研究以單塔四步驟變溫吸附程序及單塔三步驟變壓程序，進行較小型發電廠煙道氣中CO2的捕獲模擬，其進料組成為15.03%之CO2與84.97%的N2，所使用的吸附劑為依台電綜合研究所配方製備的聚苯胺固態CO2吸附劑，此吸附劑只吸附CO2，N2則為不吸附氣體。其吸附劑之吸附量為利用微量天平取得CO2飽和吸附量，以Langmuir-Freundlich isotherm吸附模式來回歸實驗數據，並進行突破曲線驗證以得到線性驅動力質傳係數。經過不同的操作變因探討以取得最佳的操作條件，以期將CO2濃度提升至90%以利之後封存，減少溫室氣體的排放。
模擬程式中使用了method of lines結合upwind differences和cubic spline approximation，再以ODEPACK套裝軟體中之LSODE程式對時間作積分，估計出下段時間的濃度、溫度及壓力，之後一直重複循環計算到系統達到週期性穩態為止。
經過變因探討後得到的最佳程序為單塔三步驟(含氮氣沖洗)變壓吸附程序，最佳操作條件為進料壓力4.0 atm、同向減壓壓力1.0 atm、逆向減壓壓力0.1 atm、塔長 550 cm、進料時間400 s、同向減壓時間30s及沖洗時間450 s，在此條件下其結果為CO2濃度91.77%，回收率為91.08%，捕捉每噸二氧化碳在絕熱壓縮或膨脹情況下所需能耗為1.04GJ/ton CO2。

摘要(英)

In this simulation study, there are two adsorption process, one-bed four-step temperature swing adsorption (TSA) and one-bed three-step pressure swing adsorption (PSA) which are utilized to separate CO2 and N2 from small size power plant flue gas(15.03% CO2, 84.97% N2) with solid polyaniline sorbent. The adsorption capacity of sorbent was measured by the Micro-Balance Thermo D-200 to obtain adsorption equilibrium data of CO2, CO2 is the only adsorbate. Then Langmuir-Freundlich isotherm model is used to establish the equilibrium isotherms by regression. After the isotherm regression, the verification of breakthrough curves are implemented to determine mass transfer coefficient, . After the process operation variables discussion, the optimal conditions are obtained to concentrate CO2 above 90% purity for storage to reduce the emission of green-house-gases.
The method of lines is utilized, combined with upwind differences, cubic spline approximation and LSODE of ODEPACK software to solve the problem. The concentration, temperature, and adsorption quantity in the bed are integrated with respect to time by LSODE of ODEPACK software. The simulation is stopped when the system reaches a cyclic steady state.
After the variables discussion, the best process is one-bed three-step PSA process with nitrogen purge and the best operating condition is feed pressure 4.0 atm, co-current depressurization pressure 1.0 atm, vacuum pressure 0.1 atm, bed length 550 cm and step time at 400, 30 and 450 s. The results of the best operating condition are 91.77% purity and 91.08% recovery of CO2 with an energy consumption of 1.04 GJ/tonCO2 at adiabatic compression and expansion conditions.

關鍵字(中)

★ 變溫吸附
★ 變壓吸附
★ 二氧化碳捕獲
★ 煙道氣

關鍵字(英)

★ temperature swing adsorption
★ pressure swing adsorption
★ CO2 capture
★ flue gas

論文目次

摘要 i
ABSTRACT ii
致謝 iv
目錄 v
圖目錄 viii
表目錄 xi
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 6
2-1-3 變壓吸附基本操作步驟 7
2-2 文獻回顧 9
2-2-1 變壓吸附程序之發展及改進 9
2-2-2 理論之回顧 13
2-2-3 利用吸附程序處理煙道氣之相關文獻 15
第三章、理論 21
3-1 基本假設 22
3-2 統制方程式 23
3-3 吸附平衡關係式 27
3-4 參數推導 28
3-4-1 聚苯胺固態CO2吸附劑對CO2的吸附熱 28
3-4-2 軸向分散係數 29
3-4-3 熱傳係數 31
3-5 邊界條件與流速 33
3-5-1 邊界條件與節點流速 33
3-5-2 閥公式 34
3-6求解步驟 35
第四章、製程描述 38
4-1 突破曲線製程 39
4-2 單塔變溫吸附製程 40
4-3 單塔變壓吸附製程 42
4-4 氣體性質與吸附參數 46
4-5 程式驗證 50
第五章、數據分析與結果討論 54
5-1 單塔變溫吸附程序之模擬 54
5-1-1 吸附溫度對單塔變溫吸附程序之影響 56
5-1-2 脫附溫度對單塔變溫吸附程序之影響 59
5-1-3 進料時間對單塔變溫吸附程序之影響 62
5-1-4 進料時間對單塔變溫吸附程序之影響(固定P/F ratio) 65
5-2 單塔變壓吸附程序之模擬 68
5-2-1 單塔三步驟變壓程序之變因探討 70
5-2-1-1 進料壓力對單塔三步驟變壓吸附程序之影響 70
5-2-2 單塔三步驟(含氮氣沖洗)變壓程序之變因探討 74
5-2-2-1 進料壓力對單塔三步驟變壓吸附程序之影響 74
5-2-2-2 逆向減壓壓力對單塔三步驟變壓吸附程序之影響 78
5-2-2-3 吸附塔塔長對單塔三步驟變壓吸附程序之影響 83
5-2-2-4 進料時間對單塔三步驟變壓吸附程序之影響 87
5-3 最佳結果討論 91
5-4 能耗之計算 93
第六章、結論 95
符號說明 97
參考文獻 101
附錄A、流速之估算方法 107
附錄B、各數據詳細資料 111
附錄C、吸附塔內溫度變化圖 120

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指導教授

周正堂(Cheng-tung Chou)

審核日期

2013-12-31

推文