以變壓吸附法濃縮己二酸工廠尾氣中氧化亞氮之模擬

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姓名

陳俊名(Chun-min 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

以變壓吸附法濃縮己二酸工廠尾氣中氧化亞氮之模擬
(Concentrating Nitrous Oxide from Flue Gases of an Adipic Acid Plant by Pressure Swing Adsorption Process)

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摘要(中)

本研究以變壓吸附程序處理己二酸工廠的尾氣，使得濃縮後的氧化亞氮可以再進行下一步驟的反應而成為製造己二酸的原料。本研究的設計根據Dolan et al.專利中的Case study為比對組，即吸附塔塔頂出去的氧化亞氮濃度低於2.5%，而塔底回收的氧化亞氮純度高於66.6%且回收率大於95%。
本研究使用的吸附劑為商用吸附劑5A沸石。研究一開始先以實驗數據中各氣體成份對吸附劑的平衡吸附量進行迴歸，以取得平衡吸附曲線的參數。之後經由理論計算出線性驅動質傳係數，並與突破曲線實驗和脫附實驗做驗證，發現脫附實驗與模擬不吻合因此對於脫附時線性驅動質傳係數做調整。再將所建立好的模擬程式與單塔四步驟程序實驗做驗證，以證明脫附時線性驅動質傳係數同時也驗證程式的可靠度。
最後以雙塔八步驟變壓吸附程序進行模擬，並藉由探討不同的操作變因如吸附塔塔長、進料壓力、真空壓力以及各步驟時間，尋求最適化的操作條件，及最適化操作條件為塔長100 cm，進料壓力2.0 atm，真空壓力0.05 atm高壓吸附時間260 s，同向減壓時間20 s，逆向減壓時間150 s，沖洗時間50 s，弱吸附氣加壓時間20 s。。其最適化的結果為塔頂氧化亞氮濃度2.4%；塔底氧化亞氮純度70.6%、回收率95.9%。

摘要(英)

This research studies concentrating nitrous oxide from the flue gases of an adipic acid plant by pressure swing adsorption (PSA) process, so that the concentrated nitrous oxide can be reacted to become the raw materials of producing adipic acid. The targets of this study are to compare to the case study of the patent which was published by Dolan et al. Those are the purity of nitrous oxide from the top effluent gases smaller than 2.5%, and the purity of nitrous oxide from the bottom product higher than 66.6% and recovery higher than 95%.
Commercialized zeolite 5A 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 were calculated by theory and verified by breakthrough curve and desorption experiment. We found that the simulation were not well fitted with desorption experiment, so we adjusted the value of parameters of desorption rate to fit the experiment. Then we verified the simulation program and the value of parameters of desorption rate by a single-bed four-step process experiment. The agreement is quite good.
In the end of this study, a dual-bed eight-step PSA process is studied. The optimal operating conditions can be obtained by assessing different operating variables such as bed length, feed pressure, vacuum pressure, and the time of each step. The results of optimal operating conditions are 70.6% purity and 95.9% recovery of nitrous oxide at bottom and 2.4% purity of nitrous oxide at top.

關鍵字(中)

★ 變壓吸附
★ 氧化亞氮
★ 製程模擬

關鍵字(英)

★ Pressure Swing Adsorption
★ Nitorus Oxide
★ Process simulation

論文目次

摘要 i
ABSTRACT ii
誌謝 iv
目錄 v
圖目錄 ix
表目錄 xvi
第一章、緒論 1
第二章、簡介及文獻回顧 6
2-1 吸附之簡介 6
2-1-1 吸附基本原理 6
2-1-2 吸附劑及其選擇性 8
2-1-3 變壓吸附基本操作步驟 9
2-2 文獻回顧 11
2-2-1 PSA程序之發展與改進 11
2-2-2 理論之回顧 14
2-3 研究背景與目的 15
第三章、理論 19
3-1 基本假設 20
3-2 統制方程式 21
3-3 吸附平衡關係式 26
3-3-1 等溫吸附平衡關係式 26
3-3-2 吸附熱關係式 27
3-4 參數推導 28
3-4-1 線性驅動質傳係數 28
3-4-2 軸向分散係數 31
3-4-3 熱傳係數 33
3-5 邊界條件與流速 35
3-5-1 邊界條件與節點流速 35
3-5-2 閥公式 36
3-6 求解步驟 37
第四章、平衡吸附曲線與吸脫附曲線 40
4-1 吸附平衡(Adsorption Equilibrium) 41
4-1-1 氣體與吸附劑性質 41
4-1-2 等溫平衡吸附曲線(Isotherm) 43
4-2 吸附動力學(Adsorption kinetics) 46
4-2-1 線性驅動質傳係數計算 46
4-2-2 突破曲線模擬驗證 49
4-2-3 脫附實驗模擬驗證 55
第五章、製程描述 61
5-1 單塔四步驟變壓吸附程序 62
5-2 雙塔八步驟變壓吸附程序 64
第六章、數據分析與結果討論 67
6-1 單塔四步驟變壓吸附程序驗證 67
6-1-1 高壓吸附時間(2nd step time)對單塔四步驟PSA製程之影響 ………………………………………………………………...69
6-1-2 進料壓力對單塔四步驟PSA製程之影響 77
6-2 雙塔八步驟變壓吸附程序之模擬 85
6-2-1 塔長對雙塔八步驟PSA製程之影響 88
6-2-2 進料壓力對雙塔八步驟PSA製程之影響 93
6-2-3 真空壓力對雙塔八步驟PSA製程之影響 98
6-2-4 高壓吸附時間(2nd/6th step time)對雙塔八步驟PSA製程之影響 ……………………………………………………………….103
6-2-5 沖洗時間(3rd/7th step time)對雙塔八步驟PSA製程之影響 ……………………………………………………………….108
6-2-6 同向減壓時間(1st/5th step time)對雙塔八步驟PSA製程之影響 ……………………………………………………………….113
6-2-7 弱吸附氣加壓時間(4th/8th step time)對雙塔八步驟PSA製程之影響 119
6-3 最適化結果討論 124
第七章、結論 126
符號說明 128
參考文獻 133
附錄A、流速之估算方法 137
附錄B、模擬結果數據 141
附錄C、最適操作條件之塔內壓力變化圖 148
附錄D、最適操作條件之塔內溫度變化圖 149
附錄E、最適操作條件之塔內氣相濃度變化圖 150

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指導教授

周正堂、楊閎舜(Cheng-tung Chou Houng-sung Yang)

審核日期

2015-7-28

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