利用變壓吸附從煉鋼廠尾氣中回收一氧化碳

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姓名

陳芊涵(Chien-Han 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

利用變壓吸附從煉鋼廠尾氣中回收一氧化碳
(Recovery of carbon monoxide from steel industry exhaust using pressure swing adsorption)

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摘要(中)

在煉鋼過程中會產生轉爐氣 (LDG)、高爐氣 (BFG) 和煉焦爐氣(COG)。前兩者具有較高含量的一氧化碳(CO)，若能將一氧化碳分離純化成高純度產品，將成為石化行業循環經濟極具潛力的原料。
本研究採用兩階段雙塔六步驟變壓吸附程序(pressure swing adsorption, PSA)來分離純化一氧化碳，模擬進料為轉爐氣和高爐氣時的氣體分離結果，期望能獲得純度95%以上的一氧化碳。根據文獻中所提到PU-1吸附劑對一氧化碳有較好的吸附效能，並於CO/N2的選擇性較好，對CO/CO2的選擇性較低。轉爐氣和高爐煤氣主要氣體組成為H2、N2、CO2和CO。因此，第一階段 PSA使用沸石5A將二氧化碳先進行分離，以提高氣體組成中的氮氣、一氧化碳含量，再於第二階段PSA中以PU-1將第一階段產物進行分離純化，獲得高濃度之一氧化碳。
本研究為獲得純度95%以上之一氧化碳，利用實驗設計(design of experiments, DOE)找尋PSA程序的最佳化操作條件，並設計高壓吸附壓力、同向減壓壓力、抽真空壓力、步驟1/4時間、步驟2/5時間、步驟3/6時間為討論的變因，進行兩水準的全因子設計，經回歸分析找到最佳化操作條件後，從轉爐氣中可獲得98.75%純度的一氧化碳且回收率達90.89%，而高爐氣則為獲得純度95.99%產品下，回收95.67%的一氧化碳。

摘要(英)

The Linz-Donawitz converter gas (LDG), blast furnace gas (BFG) and coke oven gas (COG) are important secondary energy components during the steelmaking process in iron and steel industry. The first two contain higher levels of carbon monoxide (CO). If CO can be separated and concentrated into high-purity products, it can become a highly potential raw material in petrochemical industry of circular economy. The mixed gas composition in this study focused on LDG and BFG is considered a quaternary mixtures of H2, N2, CO2 and CO with different concentrations.
In this research, we adopted a two-stage process with two-column six-step pressure swing adsorption (PSA) procedure to separate and purify CO by using two types of adsorbents of zeolite 5A and PU-1. The PU-1 adsorbent was reported with better efficiency of adsorption for CO, better selectivity for CO/N2, but lower selectivity for CO/CO2.The first-stage PSA used zeolite 5A to remove most of the CO2 from LDG and BFG. The second-stage PSA used PU-1 to obtain high CO concentration in the final product.
In order to obtain more than 95% purity of CO, this study uses the design of experiments (DOE) to predict the optimal operating conditions for the PSA process. The two-level full factorial design was discussed with adsorption pressure, cocurrent depressurization pressure, vacuuming pressure, step 1/4 time, step 2/5 time, and step 3/6 time as controlled parameters.
After simulation of the PSA process at the optimal operating conditions predicted by DOE, the final product of CO is 98.75% purity with 90.89% recovery from LDG, and 95.99% CO purity with 95.67% recovery from BFG.

關鍵字(中)

★ 變壓吸附
★ 一氧化碳
★ 二氧化碳

關鍵字(英)

★ pressure swing adsorption
★ CO
★ CO2
★ carbon monoxide
★ carbon dioxide

論文目次

摘要 i
ABSTRACT ii
致謝 iii
目錄 iv
圖目錄 viii
表目錄 x
第一章緒論 1
第二章文獻回顧 4
2-1　　吸附(Adsorption) 4
2-1-1　吸附簡介 4
2-1-2　吸附劑與其選擇性 5
2-1-3　吸附程序 7
2-1-4　突破曲線 8
2-2　　變壓吸附程序(Pressure Swing Adsorption, PSA) 10
2-2-1　變壓吸附程序之發展與改進 10
2-2-2　理論回顧 14
2-3　　一氧化碳分離之回顧 16
第三章假設與理論 18
3-1　　基本假設 18
3-2　　統制方程式 19
3-3　　吸附平衡關係式 23
3-3-1　等溫吸附平衡關係式 23
3-3-2　質傳驅動力模式(Driving Force Model) 24
3-3-3　吸附熱關係式 24
3-4　　參數推導 25
3-4-1　軸向分散係數(Axial dispersion coefficient) 25
3-4-2　熱傳係數 27
3-4-3　線性驅動力質傳係數 29
(Mass transfer coefficient of linear driving force) 29
3-5　　邊界條件與流速 32
3-5-1　邊界條件與節點流速 32
3-5-2　閥公式 33
3-6　　求解步驟 34
第四章模擬程序驗證 37
4-1　　等溫吸附實驗 37
4-1-1　實驗裝置 37
4-1-2　實驗步驟 42
4-1-3　天平校正 43
4-1-4　空白校正 44
4-1-5　等溫平衡吸附曲線 46
4-1-6 實測吸附劑能力比較 50
4-2　　突破曲線實驗 51
4-2-1　實驗裝置 51
4-2-2　突破實驗操作步驟 53
4-3　　模擬驗證 54
第五章轉爐氣之兩階段雙塔六步驟分離程序 56
5-1　　吸附劑選擇 56
5-2　　程序及模擬參數介紹 62
5-3　　模擬結果與分析 66
5-4　　以實驗設計求各響應最佳化結果 69
5-4-1　第一階段CO2-PSA實驗設計之最佳化結果 70
5-4-2　以模擬程序驗證第一階段CO2-PSA之最佳化結果 77
5-4-3　第二階段CO-PSA實驗設計之最佳化結果 79
5-4-4　以模擬程序驗證第二階段CO-PSA之最佳化結果 85
第六章高爐氣之兩階段雙塔六步驟分離程序 87
6-1　　吸附劑選擇 87
6-2　　程序及模擬參數介紹 90
6-3　　模擬結果與分析 91
6-4　　以實驗設計求最佳化結果 94
6-4-1　第一階段CO2-PSA實驗設計之最佳化結果 95
6-4-2　以模擬程序驗證第一階段CO2-PSA之最佳化結果 101
6-4-3　第二階段CO-PSA實驗設計之最佳化結果 103
6-4-4　以模擬程序驗證第二階段CO-PSA之最佳化結果 109
第七章結論 111
符號說明 113
參考資料 117
附錄 122
附錄A、流速之估算方法 122
附錄B、等溫吸附數據 126
附錄C、鋼瓶成分 132

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指導教授

周正堂(Cheng-Tung Chou)

審核日期

2022-9-5

推文