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研究生: 魏泓煜
Hong-yu Wei
論文名稱: 碳酸二乙酯反應蒸餾系統之設計與控制
Design and Control of Diethyl Carbonate Reactive Distillation Process
指導教授: 錢義隆
I-Lung Chien
口試委員: 周宜雄
Yi-Shyong Chou
汪上曉
Shang-Hsiao Wong
學位類別: 碩士
Master
系所名稱: 工程學院 - 化學工程系
Department of Chemical Engineering
論文出版年: 2010
畢業學年度: 98
語文別: 中文
論文頁數: 143
中文關鍵詞: 碳酸二甲酯碳酸二乙酯反應蒸餾設計與控制
外文關鍵詞: dimethyl carbonate, diethyl carbonate, reactive distillation, design and control
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  • 本研究以碳酸二甲酯與乙醇進行酯類置換反應,產製生物可分解之綠色化學品碳酸二乙酯及另一有用的甲醇化學品為研究的重點。碳酸二乙酯是一種工業界重要的溶劑和中間體用來取代光氣以製備norfloxacin,norfloxacin是一個廣泛被使用的抗生素。碳酸二乙酯也能用來製備其他藥物,如苯巴比妥(一種鎮靜催眠劑)。碳酸二乙酯同時也是在肥料、農藥、及聚合工業中一種重要的反應物,並在鋰離子電池中廣泛的被用做電解液。本反應系統中有兩個可逆反應,會先產生中間體碳酸甲乙酯後才反應為碳酸二乙酯。以往的文獻只有討論到碳酸二乙酯的製造。如Mueller and Kenig(2007)和Luo and Xiao(2001)都只有描述了碳酸二乙酯能從反應蒸餾塔塔底得到,並未能探討整廠製程最佳設計,以及如何控制此製程。在本年度的計畫中,我們先使用Aspen plus進行穩態模擬,研究中將探討從反應到分離之完整程序,並以最小總年度成本(TAC)為目標,先得到反應蒸餾塔最適化之穩態設計及操作條件;再接著探討若後段分離製程採用簡單蒸餾方式的年度總預算,將反應蒸餾塔與簡單蒸餾塔之年度總預算相加,進而將其整合為整廠最適化之穩態設計。再來討論當最適化反應蒸餾塔加上前置反應器後之影響,最後則探討傳統反應器製程,並比較此三種系統的優劣。本研究中亦會探討整廠製程之控制策略,期能在各類干擾下仍能保持產物的純度。最後在產量增減之變化下,本研究提供了一個溫度控制器設定點的改變以期能完美的控制住產量增減時各產物流之純度。


    A reactive-distillation system to produce diethyl carbonate (DEC) and methanol (MeOH) from dimethyl carbonate (DMC) and ethanol (EtOH) via consecutive two trans-esterification reactions is proposed in this study. Kinetic model parameters from Mueller and Kenig (2007) are used in this study. Suitable thermodynamic model parameters from regressions of experimental data are also established to describe the vapor-liquid equilibrium behavior of this system. Optimal process design and operating conditions are obtained by minimizing total annual cost (TAC). The distillate of the reactive-distillation column is a mixture of ethanol and methanol. In order to recover the excess EtOH to be recycled to the reactive-distillation column, this study using simple distillation to separate this mixture. Then compare between the optimal reactive-distillation and optimal reactive-distillation with a pre-reactor. After that, compare between conventional reactor with separation system and reactive-distillation system. Furthermore, a simple control strategy is proposed with only one tray temperature control loop in each column of the overall system. The proposed control strategy works effectively to hold the product compositions despite feed flow rate and feed composition changes. A set-point temperature adjustment scheme is proposed to maintain the purity of product composition when throughput change .

    致謝 Ⅰ 中文摘要 Ⅱ 英文摘要 IV 目錄 V 圖目錄 VII 表目錄 XV 第一章、 緒論 1 1.1前言 1 1.2文獻回顧 4 1.2.1反應蒸餾塔之程序分析 4 1.2.2 碳酸二乙酯反應蒸餾系統 5 1.2.3 醚類與酯類合成之反應蒸餾塔設計 6 1.2.4反應蒸餾塔之控制策略 8 1.3研究動機 9 1.4組織章節 11 第二章、 熱力學與動力學模式 12 2.1前言 12 2.2熱力學模式建立與參數 13 2.3蒸餘曲線圖(RCM) 22 2.4動力學模式建立與參數 27 第三章、 程序最適化設計 30 3.1前言 30 3.2碳酸二乙酯製程反應蒸餾塔設計 31 3.2.1碳酸二乙酯製程反應蒸餾塔設計概念 31 3.2.2碳酸二乙酯製程反應蒸餾塔設計概念 35 3.2.3碳酸二乙酯製程反應蒸餾塔與分離塔之最適化流 程設計 37 3.2.4碳酸二乙酯反應蒸餾塔製程進料位置之影響 53 3.2.5碳酸二乙酯製程反應蒸餾塔加上前置反應器之設 計概念 60 3.2.6碳酸二乙酯製程反應蒸餾塔加上前置反應器之設 計流程 61 3.3碳酸二乙酯傳統反應器製程系統設計 74 3.3.1碳酸二乙酯製程傳統反應器設計概念 74 3.2.2碳酸二乙酯製程傳統反應器之最適化流程設計 75 3.4經濟評估 87 第四章、動態模擬 88 4.1前言 88 4.2敏感度分析 89 4.3碳酸二乙酯整廠製程控制架構 92 4.4干擾排除 95

    鄧耀斌,「乙酸乙酯反應器/蒸餾塔流程之設計與控制」,國立台灣科大學化學工程所碩士論文(2003) .

    郭建麟,「丙烯酸乙酯製程之設計與控制」,國立台灣科大學化學工程所碩士論文(2005)

    徐愷懌,「碳酸二甲酯反應蒸餾系統之設計與控制」,國立台灣科大學化學工程所碩士論文(2009)

    羅安妮,「碳酸二乙酯反應蒸餾系統之設計」國立台灣科大學化學工程所碩士論文(2009)

    [1] Al-Arfaj, Muhammad A., and Luyben, W. L., “Comparison of Alternative Control Structures for an Ideal Two-Product Reactive Distillation Column,” Ind. Eng. Chem. Res., 39, 9, 3298-3307,(2000)
    [2] Al-Arfaj, Muhammad A., and Luyben, W. L., “Control Study of Ethyl tert-Butyl Ether Reactive Distillation,” Ind. Eng. Chem. Res., 41, 16, 3784-3796, (2002a)
    [3] Al-Arfaj, Muhammad A., and Luyben, W. L., “Control of Ethylene Glycol Reactive Distillation Column,” AIChE. Journal, 48, 4, 905-908,(2002b)

    [4] Al-Arfaj, Muhammad A., and Luyben, W. L., “Design and Control of an Olefin Metathesis Reactive Distillation Column,” Chem. Eng. Sci., 57, 5, 715-733,(2002c)
    [5] Al-Arfaj, Muhammad A., and Luyben, W. L., “Comparative Control Study of Ideal and Methyl Acetate Reactive Distillation,” Chem. Eng. Sci., 57, 24, 5039-5050, (2002d)
    [6] Alejski, Krzsztof., and Duprat, Francoise., “Dynamic Simulation of the Multicomponent Reactive Distillation,” Chem. Eng. Sci., 51, 18, 4237-4252, (1996)
    [7] Bisowarno, Budi H., Tian, Yu-Chu., Zhao, Futao., and Tade, Moses O., “Pattern-Based Predictive Control for ETBE Reactive Distillation,” J. Proc. Cont., 13, 1, 57-67, (2003)
    [8] Bock, H., Wozny, G.., and Gutsche, B. “Design and Control of a Reaction Distillation Column Including the Recovery System,” Chem. Eng. and Proc., 36, 2, 101-109, (1997)
    [9] Buzad, George., and Doherty, M. F., “Design of Three-Component Kinetically Controlled Reactive Distillation Columns Using Fixed-Point Methods”, Chem. Eng. Sci., 49, 12, 1947-1963, (1994)
    [10] Frey, T., and Stichlmair, J., “Reactive Azeotropes in Kinetically Controlled Reactive Distillation,” Chem. Eng. Res. and Des., Trans of the Ins. of Chem. Eng., Part A, 77, 7, 613-618, (1999)
    [11] Georgiadis, M. C., Schenk, M., Pistikopoulos, E. N., and Gani, R., “The Interactions of Design, Control and Operability in Reactive Distillation Systems,” Comput. and Chem. Eng., 26, 4, 735-746, (2002)
    [12] Gmehling, J., Menke, J, Krafczyk, J., Fischer, K., “Azeotropic Data”, Germany :Wiley VCH, (2004)
    [13] Gruner, S., Mohl, K. D., Kienle, A., Gilles, E. D., Fernholz, G., and Friedrich, M., “Nonlinear Control of A Reactive Distillation Column,” Control Engineering Practice, 11, 8, 915-925, (2003)
    [14] Jianjun Peng, Thomas F. Edgar , R. Bruce Eldridge “Dynamic rate-based and equilibrium models for a packed reactive distillation column” Chemical Engineering Science, 58, 2671 – 2680, (2003)
    [15] Kenig, E. Y., Bäder, H., Górak, A., Beßling, B., Adrian, T., and Shoenmakers, H., “Investigation of Ethyl Acetate Reactive Distillation Process,” Chem. Eng. Sci., 56, 6185-6193, (2001)
    [16] Lee, J. W., Bruggemann, S., and Marquardt, W., “Shortcut Method for Kinetically Controlled Reactive Distillation Systems,“AIChE. Journal, 49, 6, 1471-1487, (2003)
    [17] Luo, H.P. and Xiao, W.D., “A Reactive Distillation Process for a Cascade and Azeotropic Reaction System: Carbonylation of Ethanol with Dimethyl Carbonate”, Chem. Eng. Sci., 56, 403-410 ,(2001)
    [18] Mahajani, S. M., and Kolah, A. K., “Some Design Aspects of Reactive Distillation Columns (RDC),” Ind. Eng. Chem. Res., 35, 12, 4587-4596, (1996)
    [19] Mahajani, S. M., “Design of Reactive Distillation Columns for Multicomponent Kinetically Controlled Reactive Systems”, Chem. Eng. Sci., 54, 10, 1425-1430, (1999)
    [20] Melles, S., Grievink, J., and Schrans, Stany M., “Optimization of the Conceptual Design of Reactive Distillation Columns,” Chem. Eng. Sci., 55, 11, 2089-2097, (2000)
    [21] Mueller, I., and Kenig, E., “Reactive Distillation in a Dividing Wall Column: Rate-Based Modeling and Simulation”, Ind. End. Chem. Res., 46, 3709-3719, (2007)
    [22] Mueller, I., Pech, C., Bhatia, D., Kenig, E.Y., Rate-based Analysis of Reactive Distillation Sequences with Different Degrees of Integration”, Chem. Eng. Sci., 62, 7327-7335, (2007)
    [23] Okasinski, Matthew J., and Doherty, M. F., “Design Method for Kinetically Controlled, Staged Reactive Distillation Columns”, Ind. Eng. Chem. Res., 37, 7, 2821-2834,(1998)
    [24] Paludetto, R., Paret, G.., and Donati, G.., “Multicomponent Distillation with Chemical Reaction. Mathematical Model Analysis,” Chem. Eng. Sci., 47, 9, 2891-2896, (1992)
    [25] Pöpken, T., Steinigeweg, S., and Gmehling, J., “Synthesis and Hydrolysis of Methyl Acetate by Reactive Distillation Using Structured Catalytic Packings: Experiments and Simulation,” Ind. Eng. Chem. Res., 40, 6, 1566-1574, (2001)
    [26] Rev, Endre, “Reactive Distillation and Kinetic Azeotropy, ” Ind. Eng. Chem. Res., 33, 9, 2174-2179, (1994)
    [27] San-Jang Wang, David S. H. Wong, and En-Ko Lee, “Control of a Reactive Distillation Column in the Kinetic Regime for the Synthesis of n-Butyl Acetate” Ind. Eng. Chem. Res., 42 (21), 5182–5194,(2003)
    [28] Schmitt, M., Hasse, H., Althaus, K., and Schoenmakers, H., “Synthesis of n-hexyl Acetate by Reactive Distillation,” Chem. Eng. Proc., 43, 397-409, (2004)
    [29] Seferlis, P., and Grievink, J., “Optimal Design and Sensitivity Analysis of Reactive Distillation Units Using Collocation Models,” Ind. Eng. Chem. Res., 40, 7, 1673-1685, (2001)
    [30] Sheng-Feng Chiang, Chien-Lin Kuo, Cheng-Ching Yu, and David S. H. Wong “Design Alternatives for the Amyl Acetate Process: Coupled Reactor/Column and Reactive Distillation” Ind. Eng. Chem. Res. , 41 (13), 3233–3246, (2002)
    [31] Smejkal, Q., and Šoóš, M., “Comparison of Computer Simulation of Reactive Distillation Using ASPEN PLUS and HYSYS Software,” Chem. Eng. Proc., 41, 413-418, (2002)
    [32] Sneesby, M. G.., Tade, Moses O., Datta, R., and Smith, T. N., “ETBE Synthesis Via Reactive Distillation. 2. Dynamic Simulation and Control Aspects,” Ind. Eng. Chem. Res., 36, 5, 1870-1881, (1997)
    [33] Sneesby, M. G.., Tade, Moses O., and Smith, T. N., “Steady-State Transitions in the Reactive Distillation of MTBE,” Comput and Chem. Eng., 22, 7-8, 879-892, (1998a)
    [34] Sneesby, M. G.., Tade, Moses O., and Smith, T. N., “Multiplicity and Pseudo-Multiplicity in MTBE and ETBE Reactive Distillation,” Chem. Eng. Res. and Des., Trans of the Ins. of Chem. Eng., Part A, 76, A4, 525-531, (1998b.)
    [35] Sneesby, M. G.., Tade, Moses O., and Smith, T. N., “Two-Point Control of a Reactive Distillation Column for Composition and Conversion,” Journal of Process Control, 9, 1, 19-31, (1999.)
    [36] Sneesby, M. G.., Tade, Moses O., and Smith, T. N., “Multi-Objective Control Scheme for an ETBE Reactive Distillation Column,’ Chem. Eng. Res. and Des., Trans of the Ins. of Chem. Eng., Part A, 78, A2, 283-293, (2000)
    [37] Song, Wei, Venimadhavan, G., Manning, J. M., Malone, M. F., and Doherty, M. F., “Measurement of Residue Curve Maps and Heterogeneous Kinetics in Methyl Acetate Synthesis,” Ind. Eng. Chem. Res., 37, 5, 1917-1928, (1998)
    [38] Taylor, R., and Krishna, R., “Modelling Reactive Distillation,” Chem. Eng. Sci., 55, 5183-5229, (2000)
    [39] Thiel, C., Sundmacher, K., and Hoffmann, U., “Residue Curve Maps for Heterogeneously Catalysed Reactive Distillation of Fuel Ethers MTBE and TAME,” Chem. Eng. Sci., 52, 6, 993-1005, (1997)

    參考文獻 115

    附錄A 121

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