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| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 黃孝平 | |
| dc.contributor.author | Yu-De Lin | en |
| dc.contributor.author | 林禹德 | zh_TW |
| dc.date.accessioned | 2021-06-13T04:31:39Z | - |
| dc.date.available | 2006-07-24 | |
| dc.date.copyright | 2006-07-24 | |
| dc.date.issued | 2006 | |
| dc.date.submitted | 2006-07-19 | |
| dc.identifier.citation | [中 文]
[1] 鄭貞茂，「高分子工業年鑑」，工硏院經資中心，新竹縣，2-6-65頁 (2003)。 [2] 陳毅偉，「異相反應蒸餾系統的設計與控制」，國立臺灣大學化學工程學硏究所碩士論文 (2004)。 [3] 賴一寬，「共沸進料之反應蒸餾程序設計 : 乙酸乙酯及乙酸異丙酯」，國立臺灣大學化學工程學硏究所碩士論文 (2005)。 [英 文] [4] Al-Arfaj, M. A.; Luyben, W. L., “Effect of Number of Fractionating Trays on Reactive Distillation Performance.” AIChE J., 46(12), 2417 (2000). [5] Al-Arfaj, M. A.; Luyben, W. L., “Comparison of Alternative Control Structures for an Ideal Two-Product Reactive Distillation Column.” Ind. Eng. Chem. Res., 39(9), 3298 (2000). [6] Barbosa, D.; Doherty, M. F., “Simple Distillation of Homogeneous Reactive Mixtures.” Chem. Eng. Sci., 43(3), 541 (1988). [7] Chen, F.; Huss, R. S.; Malone, M. F.; Doherty, M. F., “Simulation of Kinetic Effects in Reactive Distillation.” Comput. Chem. Eng., 24(11), 2457(2000) [8] Douglas, J. M., Conceptual design of chemical processes, McGraw-Hill, New York, USA (1998). [9] Doherty, M. F.; Buzad, G., “Reactive Distillation by Design.” Chem. Eng. Res. Des, 70(A5), 448 (1992). [10] Doherty, M. F. and Malone, M. F., Conceptual Design of Distillation Systems, McGraw-Hill, New York, USA (2001). [11] Fuchigami,Y., ” Hydrolysis of Methyl Acetate in Distillation Column Packed with Reactive Packing of Ion Exchange Resin.” J. Chem. Eng. Jpn, 23(3), 354 (1990). [12] Gmehling, J.; Menke, J.; Krafczyk, J.; Fischer, K., Azeotropic Data, Weinheim : Wiely-VCH, Germany (2004). [13] Guttinger, T. E.; Morari, M., “Predicting Multiple Steady States in Equilibrium Reactive Distillation. 1. Analysis of Nonhybrid Systems.” Ind. Eng. Chem. Res., 38(4), 1633 (1999). [14] Guttinger, T. E.; Morari, M., “Predicting Multiple Steady States in Equilibrium Reactive Distillation. 2. Analysis of Hybrid Systems.” Ind. Eng. Chem. Res., 38(4), 1649 (1999). [15] Han, S. J.; Jin, Y.; Yu, Z. Q., “Application of a Fluidized Reaction Distillation Column for Hydrolysis of Methyl Acetate.” Chemical Engineering Journal, 66(3), 227 (1997). [16] Hoyme, C. A.; Holcomb, E. F., “Reactive Distillation Process for Hydrolysis of Esters.” U.S. Patent 6518465 (2003). [17] Hung, S. B.; Lee, M. J.; Tang, Y. T.; Chen, Y. W.; Lai, I. K.; Hung, W. J.; Huang, H. P.; Yu, C. C., “Control of Different Reactive Distillation Configurations.” AIChE J., 52(4), 1423 (2006). [18] Jacobs, R.; Krishna, R., “Multiple Solutions in Reactive Distillation for Methyl Tert-Butyl Ether Synthesis.” Ind. Eng. Chem. Res., 32(8), 1706 (1993). [19] Kaymak, D. B.; Luyben, W. L., “Effect of the Chemical Equilibrium Constant on the Design of Reactive Distillation Columns.” Ind. Eng. Chem. Res., 43(14), 3666 (2004). [20] Kim, K.J. ; Roh, H. D., “Reactive Distillation Process and Equipment for the Production of Acetic Acid and Methanol from Methyl Acetate Hydrolysis.” U.S. Patent 5770770 (1998). [21] Lee, M. M., “Method and Apparatus of Methyl Acetate Hydrolysis.” U.S. Patent 20020183549A1 (2002). [22] Luyben, W. L.; Tyréus, B. D.; Luyben, M. L. Plantwide Process Control, McGraw-Hill: New York(1999). [23] Luyben, W. L.; Pszalgowski, K. M.; Schaefer, M. R.; Siddons, C., “ Design and Control of Conventional and Reactive Distillation Processes for the Production of Butyl Acetate.” Ind. Eng. Chem. Res., 43(25), 8014 (2004). [24] Malone, M. F. and Doherty, M. F., “Reactive Distillation.” Ind. Eng. Chem. Res., 39(11), 3953 (2000) [25] Nijhuis, S.A.; Kerkhof, F. P. J. M.; Mak, A. N. S. “Multiple Steady States During Reactive Distillation of Methyl Tert-Butyl Ether.” Ind. Eng. Chem. Res., 32(11), 2767 (1993). [26] Okasinski, M. J.; Doherty, M. F., “Design Method for Kinetically Controlled, Staged Reactive Distillation Columns.” Ind. Eng. Chem. Res., 37(7), 2821 (1998). [27] Pöpken, T., Götze, L.; Gmehling, J., “Reaction Kinetics and Chemical Equilibrium of Homogeneously and Heterogneously Catalyzed Acetic Acid Esterification with Methanol and Methyl Acetate Hydrolysis.” Ind. Eng. Chem. Res., 39(7), 2601 (2000). [28] Pöpken, T.; Steinigeweg, S.; Gmehling, J., ”Synthesis and Hydrolysis of Methyl Acetate by Reactive Distillation Using Structured Catalytic Packings: Experiments and Simulation.” Ind. Eng. Chem. Res., 40(6), 1566 (2001). [29] Qiu, T.; Ma, P. S.; Wang, L. E.; Zheng, H. D., “Determination and correlation of liquid-liquid equilibrium data for the methyl acetate-methanol-water ternary system,” Huaxue Gongcheng/Chemical Engineering (China), 32(4), 62 (2004). [30] Ryan, P J.; Doherty, M. F., “Design/optimization of ternary heterogeneous azeotropic distillation sequences.” AIChE J., 35(10), 1592 (1989). [31] Sneesby, M. G.; Tade, M. O.; Smith, T. N., “Two-point Control of a Reactive Distillation for Composition and Conversion.” Journal of Process Control, 9(1), 19 (1999). [32] Song, W.; Venimadhavan, G.; Manning, J. M.; Malone, M. F.; Doherty, M. F., “Measurement of Residue Curve Maps and Heterogeneous Kinetics in Methyl Acetate Synthesis.” Ind. Eng. Chem. Res., 37(5), 1917 (1998). [33] Sundmacher, K. and Kienle, A., Reactive Distillation：Status and Future Directions, Wiley-VCH Verlag GmbH & Co. KGaA：Weinheim, Germany (2003). [34] Tang, Y. T.; Chen, Y. W.; Huang, H. P.; Yu, C. C.; Hung, S. B.; Lee, M. J., “Design of Reactive Distillations for Acetic Acid Esterification.”, AIChE J., 51(6), 1683 (2005). [35] Wang, J.; Ge, X.; Wang, Z.; Jin, Y., ” Experimental Studies on the Catalytic Distillation for Hydrolysis of Methyl Acetate,” Chem. Eng. Technol, 24(2), 155（2001）. [36] Xiao, J.; Liu, J.; Li, J.; Jiang, X.; Zhang, Z., “Increase MeOAc Conversion in PVA Production by Replacing the Fixed Bed Reactor with a Catalytic Distillation Column.” Chem. Eng. Sci, 56(23), 6553 (2001). [37] Xu, Z. P.; Chuang, K. T., “Kinetics of acetic acid esterification over ion exchange catalysts.” Can. J. Chem. Eng, 74(4), 493 (1996). | |
| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/33260 | - |
| dc.description.abstract | 本研究針對聚乙烯醇工廠所產生的乙酸甲酯(MeAc)，以反應蒸餾塔將其水解為更具價值的乙酸及甲醇，改善傳統製程中低轉化率的缺點。系統由一個反應蒸餾塔、兩個分離塔及一迴流股組成。乙酸甲酯與過量的水進行反應，以Amberlyst 15離子交換樹脂作為異相觸煤。由於水解反應速度慢且乙酸甲酯沸點低，反應蒸餾塔操作上須採塔頂全回流方式以達到高轉化率，避免後續分離程序中醇酯共沸物形成。塔底產物送入第二根塔進行分離，於塔底得到乙酸，產品規格為99mol%。塔頂產物送入第三根，塔頂得到甲醇，塔底大量的水迴流至反應蒸餾塔中。
為了模擬真實工廠操作，將乙酸甲酯進料條件分為純進料與共沸進料(60mol% MeAc)系統，並藉由計算年總成本(TAC)進行最適化設計。水解乙酸甲酯系統為迴流程序，單元之間操作上有其關聯性。在反應與分離程序成本間，應取得一平衡點，以符合最經濟的系統架構。在最適設計步驟中，我們發現兩個最重要的變數：迴流股流量(水過量幅度)及第二根塔頂乙酸規格(乙酸與水之間有狹點存在)。 在系統動態方面，我們提出三種控制架構(CS1~CS3)，包含溫度控制與濃度控制。為了確保兩產品組成均達到規格，在控制架構中，以第三根塔底液位控制新鮮水入料量，於系統中維持化學計量平衡。在溫度控制下將造成產品組成偏差；而濃度控制雖然響應較慢，但最終產品濃度符合規格，由模擬結果可知這些架構對於進料條件擾動有良好的排除效果。 | zh_TW |
| dc.description.abstract | This work explores the hydrolysis of methyl acetate (MeAc) from the PVA plant, and produce high purity acetic acid and methanol by reactive distillation which improves the conversion of MeAc in conventional processes. The process consists of one reactive distillation column, two distillation columns and one recycle stream. MeAc is reacted with excess water, and we use Amberlyst 15 ion-exchange resin as heterogeneous catalyst. Due to low reaction rate and methyl acetate is a light component, total reflux operation in reactive column is required to reach high conversion of MeAc and avoid azeotropes in the separation process. The bottoms flow from the reactive column is fed to the second column, which produces acetic acid with 99mol% purity in the bottom and the distillate goes to the third column. The methanol product comes out from the top of the third column and a water-rich bottom stream is recycled back to the reactive column.
In order to simulate real situation, both pure feed and azeotropic feed (60mol% MeAc) systems are considered in optimum design based on total annual cost (TAC). The hydrolysis system is a recycle process, and relevance of each unit operation is strong. There should be an equilibrium between the cost of reaction and separation process to have the most economic structure. In optimal design procedure, two important design variable are identified: one is recycle flow rate (the amount of excess water) and the other is specification of acetic acid in the distillate of second column (pinch point exists between water-acetic acid system). In process dynamics, three control strategies (CS1~CS3) are studied, including temperature and composition control. The system should keep stoichiometric balance for satisfying both product specifications. Therefore, in the control structure, fresh water feed is controlled by the liquid level of the third column. Temperature control results in offsets in product composition. Although composition control has slow response, it maintains product purity close to their set points. The result shows these schemes have good performance for disturbance rejection. | en |
| dc.description.provenance | Made available in DSpace on 2021-06-13T04:31:39Z (GMT). No. of bitstreams: 1 ntu-95-R93524084-1.pdf: 1875645 bytes, checksum: a42b0bd7faca81de98ec9c98971bb57a (MD5) Previous issue date: 2006 | en |
| dc.description.tableofcontents | 致謝 I
摘要 III Abstract V 目錄 VII 圖索引 IX 表索引 XI 1. 緒論 1 1.1. 前言 1 1.2. 文獻回顧 5 1.3. 研究動機與目的 9 1.4. 組織章節 11 2. 熱力學及動力學模式 13 2.1. 前言 13 2.2. 熱力學模式 14 2.2.1 液相之熱力學模式 15 2.2.2 氣相之熱力學模式 16 2.2.3 兩相區分布之探討 17 2.2.4 乙酸甲酯反應蒸餾系統之蒸餘曲線圖分析 18 2.2.5 座標轉換系統 23 2.3. 動力學模式 25 3. 穩態設計 29 3.1. 前言 29 3.2. 水解乙酸甲酯製程 29 3.3. 最適化步驟 31 3.4. 純進料及共沸進料系統之最適化設計 34 3.4.1 反應段及汽提段板數的影響 35 3.4.2 反應蒸餾塔中進料位置的影響 37 3.4.3 分離塔中總板數與進料位置的影響 39 3.4.4 迴流量的影響 41 3.4.5 第二根塔頂乙酸規格的影響 44 3.4.6 純進料與共沸進料系統之最適化設計與比較 46 3.4.7 總結 50 3.5. 純進料及共沸進料系統溫度分佈及濃度分佈之探討 51 3.5.1 溫度分佈之探討 51 3.5.2 濃度分佈之探討 54 3.6. 系統架構對轉化率之影響 57 4. 動態模擬及控制 59 4.1. 前言 59 4.2. 控制環路設計 59 4.3. 控制架構的探討 60 4.3.1 控制架構分類(CS1~CS3) 60 4.3.2 系統所承受的干擾 61 4.4. CS1三溫度控制 61 4.4.1 開環路靈敏度分析 63 4.4.2 控制器參數調諧方法 67 4.4.3 CS1三溫度控制動態模擬結果 70 4.5. CS2三溫度控制 74 4.5.1 開環路靈敏度分析與控制器參數 75 4.5.2 CS2三溫度控制動態模擬結果 77 4.6. 溫度控制的改善 81 4.7. 二組成及一溫度控制 85 4.7.1 CS3二組成及一溫度控制動態模擬結果 85 5. 結論 89 附錄A 年總成本計算公式 91 附錄B 庫存控制環路控制器參數 93 參考文獻 94 | |
| dc.language.iso | zh-TW | |
| dc.subject | 年總成本 | zh_TW |
| dc.subject | 反應蒸餾 | zh_TW |
| dc.subject | 乙酸甲酯 | zh_TW |
| dc.subject | 水解 | zh_TW |
| dc.subject | Methyl Acetate | en |
| dc.subject | TAC | en |
| dc.subject | Hydrolysis | en |
| dc.subject | Reactive Distillation | en |
| dc.title | 水解乙酸甲酯反應蒸餾系統之設計與控制 | zh_TW |
| dc.title | Design and Control of Reactive Distillation System for Hydrolysis of Methyl Acetate | en |
| dc.type | Thesis | |
| dc.date.schoolyear | 94-2 | |
| dc.description.degree | 碩士 | |
| dc.contributor.oralexamcommittee | 余政靖,周宜雄,汪上曉,黃琦聰 | |
| dc.subject.keyword | 反應蒸餾,乙酸甲酯,水解,年總成本, | zh_TW |
| dc.subject.keyword | Reactive Distillation,Methyl Acetate,Hydrolysis,TAC, | en |
| dc.relation.page | 97 | |
| dc.rights.note | 有償授權 | |
| dc.date.accepted | 2006-07-21 | |
| dc.contributor.author-college | 工學院 | zh_TW |
| dc.contributor.author-dept | 化學工程學研究所 | zh_TW |
| 顯示於系所單位： | 化學工程學系 | |
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