利用全因子實驗設計進行三塔十二步驟真空變壓吸附法捕獲燃煤電廠1-kW煙道氣中二氧化碳之最適化研究

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林耀庭(Yao-Ting Lin) 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

利用全因子實驗設計進行三塔十二步驟真空變壓吸附法捕獲燃煤電廠1-kW煙道氣中二氧化碳之最適化研究
(Optimal investigation on carbon dioxide capture in 1-kW flue gas from coal-fired power plant by a three-bed twelve-step vacuum pressure swing adsorption using full factorial design)

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摘要(中)

面對日益嚴重的溫室效應及嚴峻的氣候變遷，減碳已蔚為國際浪潮。目前捕獲二氧化碳有多種技術。由於變壓吸附法能耗低，資本投資低等優點，因此本研究將使用該技術進行捕獲台中燃煤電廠中煙道氣的二氧化碳之模擬與實驗，並期望能使捕獲的二氧化碳純度達95 %及回收率達65 %。
本研究首先以高壓氣體吸附分析儀搭配Thermo Cahn D-200 Digital Recording Balance測量二氧化碳及氮氣在吸附劑COSMO 13X沸石之等溫吸附曲線，計算平衡選擇率確認所選用的吸附劑具有良好的分離效果，並以Langmuir-Freundlich isotherm模型對等溫吸附曲線實驗數據進行擬合得到模擬所需之參數。接著以突破曲線及三塔變壓吸附程序之實驗驗證模擬所使用之相關參數是否合理，經過試誤法(trial-and-error)得出當等溫吸附擬合曲線之修正因子為0.55時，能使模擬與實驗結果接近。
接著利用三塔十二步驟變壓吸附程序模擬兩水準六因子之全因子實驗設計，先初步找出其中三個影響較為顯著之因子，再至台中電廠進行兩水準三因子的全因子實驗設計以探討因子對於塔底二氧化碳之純度、回收率、捕獲能耗及產率之影響，並建立各響應之迴歸模型找出最適化操作條件。最後得到當實驗步驟3/7/11時間為200秒，進料壓力3.5 bar，同向減壓壓力為0.30 bar時，可以得到捕獲二氧化碳純度97.50 %、回收率68.54 %、能耗1.43 GJ/tonne of CO2及產率0.42 kg CO2/kg adsorbent∙day之最適化結果。

摘要(英)

With the concern over global warming and extreme climate change, carbon reduction has become a global trend in recent years. When it comes to carbon capture, there are several methods to deal with this. This research was concerned about carrying out pressure swing adsorption(PSA) simulation and experiments to capture carbon dioxide because of its low energy consumption and low capital investment, and aimed to capture carbon dioxide from 1-kW flue gas in Taichung coal-fired power plant with CO2 product purity reaching 95 %, and recovery reaching 65 % at the same time.
First of all, the adsorption isotherm curves of carbon dioxide and nitrogen for zeolite 13X molecule sieve were obtained by High Pressure Gas Adsorption Analyzer and Thermo Cahn D-200 Digital Recording Balance, and the equilibrium selectivity was calculated to confirm whether adsorbent has good ability to separate carbon dioxide and nitrogen.
Langmuir-Freundlich isotherm model was used to fit the adsorption experimental data in order to obtain the isotherm parameters for simulation. Furthermore, breakthrough curve and the three-bed PSA experiment were used for simulation verification. Through trial-and-error method, it was found that when the correction factor of adsorption isotherm equals to 0.55, the results of simulation and experiments can agree well.
Next, two-level six-factor full factorial design with three-bed twelve-step PSA process simulation was conducted for the sake of finding three relatively significant factors, and two-level three-factor full factorial design experiments were conducted in Taichung coal-fired power plant afterwards. Finally, the optimal operating conditions were predicted from regression model of design of experiments(DOE). After experiments at optimal operating conditions, the bottom CO2 product purity is 97.50 % with recovery 68.54 %, and energy consumption and productivity were measured to be 1.43 GJ/tonne of CO2 and 0.42 kg CO2/kg adsorbent∙day when step 3/7/11 time equaled to 200 s, adsorption pressure equaled to 3.5 bar and cocurrent depressurization pressure equaled to 0.30 bar.

關鍵字(中)

★ 變壓吸附
★ 燃煤電廠
★ 二氧化碳捕獲
★ 全因子設計

關鍵字(英)

★ pressure swing adsorption
★ coal-fired power plant
★ carbon dioxide capture
★ full factorial design

論文目次

摘要 i
ABSTRACT ii
誌謝 iv
目錄 v
圖目錄 ix
表目錄 xiii
符號說明 xv
第一章、緒論 1
第二章、簡介與文獻回顧 5
2-1 吸附之簡介 5
2-1-1 吸附基本原理 5
2-1-2 吸附劑與其選擇率 8
2-1-3 等溫吸附曲線(Adsorption isotherm) 10
2-1-4 突破曲線(Breakthrough curve) 12
2-1-5 變壓吸附程序之發展與演進 14
2-1-6 文獻回顧 18
2-1-7 研究目的 22
第三章、實驗設備與方法 23
3-1 煙道氣之氣體與實驗吸附劑 23
3-2 變壓吸附程序模擬之理論 25
3-2-1 基本假設 26
3-2-2 統制方程式 27
3-2-3 吸附平衡關係式 30
3-2-3-1 等溫吸附平衡關係式 30
3-2-3-2 質傳速率模式 31
3-2-3-3 吸附熱關係式 33
3-2-4 參數推導 34
3-2-4-1 軸向分散係數(Axial dispersion coefficient) 34
3-2-4-2 熱傳係數 36
3-2-4-3 線性驅動力質傳係數(Mass transfer coefficient of linear driving force) 38
3-2-5 邊界條件與流速 41
3-2-5-1 邊界條件與節點流速 41
3-2-5-2 閥公式 42
3-2-6 求解步驟 43
3-3 實驗儀器 45
3-3-1 等溫吸附曲線實驗 45
3-3-2 突破曲線與真空變壓吸附實驗 48
3-3-2-1 煙道氣前處理部分 48
3-3-2-2 三塔真空變壓吸附實驗部分 52
3-4 製程描述 56
3-4-1 煙道氣預處理程序 59
3-4-2 三塔真空變壓吸附程序 59
3-5 實驗步驟 62
3-5-1 等溫吸附曲線 62
3-5-2 突破曲線實驗 63
3-5-3 三塔真空變壓吸附實驗 64
3-6 實驗數據計算方法 65
3-7 實驗設計(Design of Experiments) 67
3-7-1 全因子設計(Full factorial design) 67
3-7-2 變異數分析(Analysis of Variance, ANOVA) 68
3-7-3 殘差分析圖(Residual analysis plots) 70
3-7-4 迴歸分析(Regression analysis) 71
第四章、等溫吸附曲線、突破曲線與三塔變壓吸附程序之模擬驗證 74
4-1 等溫吸附曲線模擬參數取得及驗證 75
4-2 台中電廠規模吸附塔之突破曲線模擬驗證 77
4-3 不同變壓吸附程序捕獲煙道氣二氧化碳之模擬與比較 82
4-4 三塔十二步驟變壓吸附程序捕獲煙道氣中二氧化碳之模擬驗證 87
4-5 三塔十二步驟變壓吸附模擬程序捕獲燃煤電廠煙道氣中二氧化碳之基礎條件 92
第五章、結果與討論 94
5-1 等溫吸附曲線實驗 94
5-2 燃煤電廠煙道氣突破曲線實驗 96
5-3 變壓吸附程序模擬之兩水準六因子實驗設計分析 98
5-3-1 兩水準六因子之殘差分析圖 99
5-3-2 兩水準六因子之變異數分析 100
5-4 變壓吸附程序實驗之兩水準三因子實驗設計分析 105
5-4-1 利用Lenth’s method判斷因子之顯著性 108
5-4-2 殘差分析圖、迴歸模型建立及柏拉圖 111
5-4-3 三塔十二步驟變壓吸附程序之響應最適化 119
5-4-3-1 探討塔底二氧化碳純度及回收率最大值之響應最適化 120
5-4-3-2 探討塔底二氧化碳純度及回收率僅達目標值之響應最適化 121
5-4-3-3 響應最適化結果之比較與探討 123
第六章、結論 125
參考文獻 127
附錄一、流速之估算方法 132
附錄二、三塔變壓吸附平台流程圖各元件對照表 135
附錄三、三塔變壓吸附平台流程圖元件命名法 141
附錄四、F分佈表 142
附錄五、t分佈表 143
附錄六、考慮不同因子及交互作用之殘差分析圖 144

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指導教授

周正堂(Cheng-Tung Chou)

審核日期

2022-9-7

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