使用Aspen Plus模擬連續式反應器之端羥基聚丁二烯自由基聚合和分離純化程序設計

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李丞軒(Cheng-Hsuan Li) 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

使用Aspen Plus模擬連續式反應器之端羥基聚丁二烯自由基聚合和分離純化程序設計
(Utilizing Aspen Plus to Simulate The Continuous Reactor for Hydroxyl-Terminated Polybutadiene Free Radical Polymerization and Separation Purification Process Design)

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摘要(中)

端羥基聚丁二烯(hydroxyl-terminated polybutadiene, HTPB)為一種遙爪聚合物，分子結構是由末端氫氧基，中間為不同形式的丁二烯單元所組成。HTPB具有多功能特性，常用於黏合劑、燃料和塗料等不同領域中。然而，目前國內大多數的HTPB皆仰賴國外進口，這可能會帶來一些不便，如國內外法規、原料品質不穩定和物價波動等。因此，我們希望未來能夠自主生產合格的HTPB，以降低對外部的依賴。
本研究之目的為使用Aspen Plus建立連續式製成HTPB的方法。進料方面設計兩條管線，通過改變壓力與溫度，以確保原料以液體型態進入反應器，可減少安全隱患。反應方面採用可控性高、反應機制單純的自由基聚合(free radical polymerization, FRP)，並利用真實實驗數據，計算3/8吋管塞流式反應器(3/8’’plug flow reactor, 3/8’’PFR)和微通道反應器(Microchannal reactor, MCR)的動力學參數。此外，使用Aspen Plus中內建分析工具，透過改變進料比例、反應時間、反應溫度等參數，調節HTPB的規格。在分離方面，我們使用分離器與蒸餾塔將HTPB、丁二稀和異丙醇純化，並將純化後的丁二烯與異丙醇進行循環再利用。
這項研究已成功建立了Aspen Plus快速計算動力參數之方法，並且模擬結果與真實實驗數據相當吻合，這表明在流程設計與參數計算上具有相當高的參考性。此外，我們在保持原料完全於液相的條件下，找到合適的反應參數，使轉化率達到40%，並且數均分子量保持於3000左右。通過純化後的HTPB、丁二烯與異丙醇，純度皆能達到99%以上。丁二烯與異丙醇回收率可達99%以上，且經回收再利用後，不會造成HTPB之性質改變，有效地避免原料的浪費。

摘要(英)

Hydroxyl-terminated polybutadiene (HTPB) is a telechelic polymer, with a molecular structure composed of terminal hydroxyl groups and various forms of butadiene units in the middle. HTPB possesses multifunctional characteristics and is commonly used in adhesives, fuels, and coatings across various fields. However, most HTPB used domestically is imported, which can lead to certain inconveniences, such as differences in domestic and international regulations, instability in raw material quality, and price fluctuations. Therefore, we aim to independently produce qualified HTPB in the future to reduce our reliance on external sources.
The purpose of this study is to establish a continuous process for producing HTPB using Aspen Plus. The feed design includes two pipelines that adjust pressure and temperature to ensure the materials enter the reactor in liquid form, reducing safety hazards. The reaction uses free radical polymerization (FRP), which has high controllability and a simple reaction mechanism. By utilizing actual experimental data, we calculate the kinetic parameters for a 3/8’’ plug flow reactor (3/8’’PFR) and a microchannel reactor (MCR). Additionally, we use built-in analysis tools in Aspen Plus to adjust HTPB specifications by altering parameters such as feed ratio, reaction time, and reaction temperature. In the separation process, we use separator and distillation columns to purify HTPB, butadiene, and isopropanol, and recycle the purified butadiene and isopropanol.
This study successfully established a method for quickly calculating kinetic parameters using Aspen Plus. The simulation results closely matched actual experimental data, indicating high reliability in process design and parameter calculations. Furthermore, under conditions that keep the materials entirely in the liquid phase, we found suitable reaction parameters that achieved a conversion rate of 40%, with the number-average molecular weight maintained around 3000. The purified HTPB, butadiene, and isopropanol all achieve a purity of over 99%. The recovery rates of butadiene and isopropanol are also above 99%, and their recycling does not alter the properties of HTPB, effectively preventing material waste.

關鍵字(中)

★ 端羥基聚丁二烯
★ 微通道反應器
★ Aspen plus

關鍵字(英)

★ hydroxyl-terminated polybutadiene (HTPB)
★ microchannel reactor (MCR)
★ Aspen Plus

論文目次

摘要 i
Abstract iii
致謝 v
目錄 vii
圖目錄 xi
表目錄 xv
第一章緒論 1
1-1 前言 1
1-2 研究動機 4
第二章文獻回顧 6
2-1 HTPB介紹 6
2-2 HTPB規格 9
2-2-1 數均分子量、重均分子量、分子量分佈介紹 10
2-2-2 鏈段比例介紹 11
2-2-3 產量與轉化率介紹 12
2-3 HTPB聚合方式 14
2-3-1 自由基聚合 14
2-3-2 活性陰離子聚合 16
2-3-3 開環復分解聚合 17
2-4 起始劑選擇 19
2-5 溶劑選擇 22
2-6 微流道反應器介紹 25
2-7 Aspen Plus介紹 28
第三章實驗方法及步驟 30
3-1 模擬軟體介紹 30
3-1-1 模擬軟體操作設置 30
3-2 HTPB自由基聚合反應動力學 31
3-2-1 HTPB自由基聚合反應機制 31
3-2-2 起始劑解離速率常速(kd) 32
3-2-3 反應中間體單自由基長鏈分子的濃度([RM·]) 32
3-2-4 動力學鏈長("ν" )與聚合度(Xn) 33
3-3 Aspen Plus程序設計與參數設定 35
第四章結果與討論 38
4-1 動力參數計算 38
4-2 3/8’’PFR參數模擬 40
4-2-1 初級自由基添加單體步驟(Ra)對HTPB所造成之影響 41
4-2-2 鏈增長反應速率常數(kp)與鏈終止反應速率常數(kt)之特殊關係式 42
4-2-3 動力參數校正 43
4-2-4 3/8’’PFR動力參數與模擬結果 44
4-2-5 3/8’’PFR模擬HTPB鏈段 45
4-3 MCR參數模擬 48
4-3-1 校正MCR動力參數 50
4-3-2 溫度與壓力對HTPB之影響 51
4-3-3 氣化壓力與進料流率比例關係 53
4-3-4 進料流率比例對HTPB之影響 56
4-3-5 滯留時間對HTPB之影響 59
4-3-6 比較MCR與3/8’’PFR 61
4-4 提升反應轉化率 63
4-4-1 提升MCR之反應器規格 63
4-4-2 MCR45串聯3/8’’PFR 64
4-5 分離純化之程序設計 67
4-5-1 HTPB純化分離 67
4-5-2 BD純化分離 68
4-5-3 IPA純化分離 73
4-5-4 原料循環 78
4-5-5 循環前後之反應結果 81
第五章結論與未來展望 82
第六章附錄 84
6-1 流程圖(圖3- 2)管線內部流率與組成 84
6-2 於Aspen Plus中PDI之變化 88
參考文獻 90

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指導教授

李岱洲(Tai-Chou Lee)

審核日期

2024-8-22

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