雙塔式變壓吸附法捕獲合成氣中二氧化碳之實驗設計分析

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沈珍瑜(Chen-Yu Shen) 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

雙塔式變壓吸附法捕獲合成氣中二氧化碳之實驗設計分析

相關論文

★ 利用半圓柱型吸附塔進行變壓吸附程序分離空氣之模擬研究	★ 利用熱交換吸附塔結構設計之變壓吸附程序分離空氣製氧之模擬研究
★ 合成氣經富氧燃燒後利用雙塔變壓吸附程序純化二氧化碳之實驗	★ 以變壓吸附程序捕獲發電廠煙道氣中二氧化碳及濃縮合成氣經富氧燃燒後中二氧化碳之研究與實驗設計分析
★ 利用雙塔變壓吸附程序捕獲煙道氣中二氧化碳之實驗設計分析	★ 以變壓吸附法捕獲發電廠煙道氣中二氧化碳之模擬研究與實驗設計分析

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摘要(中)

變壓吸附程序是一種分離氣體混合物的技術，根據不同氣體成份對吸附劑吸附能力的不同，進而利用吸附選擇性的高低來篩選氣體，再搭配吸附劑在高壓利於吸附、低壓利於脫附之特性，進行高低壓循環程序達到氣體分離的目的。具有容易操作、吸附劑可再生利用等優點。本研究利用變壓吸附法將二氧化碳濃縮以利後續封存，減少二氧化碳排放至大氣中，避免溫室效應的惡化。
本研究以雙塔六步驟變壓吸附法捕獲經水煤氣轉化後之合成氣中的二氧化碳，進料氣體以41.4%二氧化碳與58.6%氮氣模擬合成氣經過水煤氣轉化後的組成。選用13X沸石作為吸附劑，並將其填入吸附塔內進行突破及脫附曲線實驗，藉由改變不同的進料壓力與溫度，觀察其對突破曲線及脫附曲線之影響，並作為後續變壓吸附程序參數探討的基礎。
為降低實驗成本，利用實驗設計分析方法探討雙塔六步驟變壓吸附程序之二氧化碳捕獲實驗，並建立兩水準之部分因子設計(fractional factorial design)，探討各操作變因（進料壓力、溫度、逆向減壓壓力、進料加壓/同向減壓時間、高壓吸附/逆向減壓時間、高壓吸附/低壓沖洗時間）對製程的影響。實驗結果發現對純度而言，進料壓力及高壓吸附/逆向減壓時間為顯著因子；對回收率而言，各因子皆不顯著。在進料壓力3.45 atm、步驟一時間140秒、步驟二時間160秒、步驟三時間20秒、抽真空壓力0.05 atm、溫度358 K之操作條件下，純度可達90.39%、回收率79.73%。
最後以逐步回歸方式建立純度、回收率與變因之模型，以此模型來進行實驗預測、製程最佳化、量產製程變異性及提供系統操作之參數決策。

摘要(英)

Pressure swing adsorption process is a technique used to separate gas mixtures according to the different adsorption capacities and selectivity toward adsorbent. Based on the property of adsorption at high pressure and desorption at low pressure, we can choose the appropriate processes to achieve the desired separation. Pressure swing adsorption process is used to concentrate carbon dioxide in order to mitigate the effects of global warming and reduce emissions.
In this study, pressure swing adsorption process is utilized to separate CO2 and N2 from syngas after water gas shift reaction. The compositions of syngas are simulated as 41.4% CO2 / 58.6% N2. To purify 41.4% CO2 with balance N2 as a captured gas mixture, two-bed six-step pressure swing adsorption process using zeolite 13X were experimentally studied.
Breakthrough curve experiments were carried out. These experimental results could be foundation of investigating pressure swing adsorption process. Two-bed pressure swing adsorption process was applied to carry out CO2 capture experiment.
The design of experiment (DOE) of two-bed six-step pressure swing adsorption process. Pressurization / cocurrent depressurization time, adsorption / countercurrent depressurization time, adsorption / purge time, feed pressure, temperature, vacuum pressure are the factors of two-level six-factor fractional factorial design to investigate the change of CO2 concentration and recovery. The analysis shows that the main effects feed pressure and adsorption / countercurrent depressurization time were significant effects for purity. CO2 with 90.39% purity and 79.73% recovery was found at pressurization / cocurrent depressurization time 140 s, adsorption / countercurrent depressurization time 160 s, adsorption / purge time 20 s, temperature 358 K, feed pressure 3.45 atm and a fixed vacuum pressure of 0.05 atm.
Finally, we build a model relating purity to factors and recovery to factors, and use a regression model to present the results of our designed experiment.

關鍵字(中)

★ 變壓吸附
★ 合成氣
★ 實驗設計
★ 二氧化碳

關鍵字(英)

★ pressure swing adsorption
★ syngas
★ design of experiment
★ CO2

論文目次

摘要 i
ABSTRACT iii
誌謝 iv
目錄 v
圖目錄 viii
表目錄 xi
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
2-2 變壓吸附法基本操作步驟 8
2-3 PSA之程序發展與改進 11
2-4 吸附劑及其選擇性 15
2-5 等溫平衡吸附曲線 18
2-6 突破曲線與脫附曲線 20
2-7 文獻回顧 22
第三章、實驗設備及方法 26
3-1 吸附劑選擇 26
3-2 突破曲線與脫附曲線實驗 28
3-2-1 實驗步驟 32
3-3 變壓吸附實驗 33
3-3-1 實驗裝置、各部規格及特性 36
3-3-2 實驗步驟 40
3-4 部分因子設計 43
第四章、實驗結果與討論 48
4-1 吸附劑選擇計算與討論 48
4-2 突破曲線實驗與脫附曲線實驗結果與討論 54
4-2-1 流速對突破曲線的影響 55
4-2-2 流速對脫附曲線的影響 57
4-2-3 塔內溫度對突破曲線的影響 59
4-2-4 塔內溫度對脫附曲線的影響 61
4-3 變壓吸附實驗之實驗設計分析 63
4-3-1 Effects plot之分析 66
4-3-2 變異數分析(Analysis of Variance, ANOVA) 71
4-3-3 主效用圖(Main effect plot)與交互作用圖(Interaction plot) 73
4-3-4 逐步回歸(Stepwise regression) 81
4-3-5 殘差分析(Residual analysis) 85
4-3-6 以模型回歸之結果與實驗值比較 91
4-3-7 模型修正 94
4-4 能耗計算 97
第五章、結論 100
參考文獻 102
附錄A、變壓吸附程序詳細數據 106
附錄B、名詞簡介 111

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指導教授

周正堂楊閎舜(Cheng-Tung Chou Hong-Sung Yang)

審核日期

2018-8-21

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