Side-by-side Chinese-English

带侧线反应精馏-渗透汽化生产乙酸乙酯集成过程模拟与分析

金浩1 陆佳伟1 汤吉海1,2 张竹修1 费兆阳1 刘清1 陈献1 崔咪芬1 乔旭1,2

(1.材料化学工程国家重点实验室南京工业大学化工学院, 江苏南京 210009)
(2.国家“江苏先进生物与化学制造协同创新中心”, 江苏南京 210009)
【知识点链接】反应精馏

【摘要】针对乙酸酯化法生产乙酸乙酯分离过程复杂、能耗大的缺点, 提出了一种带侧线反应精馏-渗透汽化 (RD-PV) 集成过程。通过反应精馏塔侧线采出和渗透汽化膜组件及时移出水分, 促进酯化反应向正反应方向进行, 在达到乙酸高转化率的同时使乙酸乙酯产品达到高纯度。研究了反应精馏塔侧线采出位置、采出比、反应段塔板数、精馏段塔板数以及膜组件个数等对年度总成本 (TAC) 的影响, 获得了TAC达到最小的过程参数。与传统双塔精馏分离过程对比, RD-PV集成过程节省能耗26.6%, 但膜材料价格对RD-PV集成过程的TAC有较大影响, 随着渗透汽化技术的成熟, 当膜材料价格低于1913 CNY·m-2时, RD-PV集成过程在经济上占据优势。

【关键词】 反应精馏;渗透汽化;集成;计算机模拟;乙酸乙酯;

【DOI】

【基金资助】 国家重点研发计划项目 (2017YFB0307304) ; 国家自然科学基金项目 (21276126, 61673205) ; 江苏省“333工程”项目 (BRA2016418) ; 江苏省“六大人才”高峰项目 (XCL-017) ; 江苏高校优势学科建设工程项目 (PAPD) ;

Simulation and analysis of a side stream reactive distillation-pervaporation integrated process for ethyl acetate production

JIN Hao1 LU Jiawei1 TANG Jihai2 ZHANG Zhuxiu1 FEI Zhaoyang1 LIU Qing1 CHEN Xian1 CUI Mifen1 QIAO Xu

(1.State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, Jiangsu, China 210009)
(2.Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM) , Nanjing, Jiangsu, China 210009)
【Knowledge Link】reactive distillation

【Abstract】Due to the complicated process and huge energy consumption of ethyl acetate production via esterification of acetic acid and ethanol, a reactive distillation and pervaporation integrated process is proposed. The byproduct water is removed from the system through the side stream of the column and membrane modules, which promotes the forward reaction and improves the purity of ethyl acetate. The effect of the process parameters on total annual cost is investigated. The parameters include side stream drawn stage, side stream flow rate ratio, reactive stages, rectifying stages and number of membrane modules. Compared with conventional double-column process, the proposed RD-PV integrated process saves 26.6% energy. Through the investigation, it is found that the price of membrane material has significant effect on the total annual cost of RD-PV integrated process. With the development of pervaporation technology, the RD-PV process would appear economically competitive, when the price of membrane material is lower than 1 913 CNY·m−2.

【Keywords】 reactive distillation; pervaporation; integration; computer simulation; ethyl acetate;

【DOI】

【Funds】 National Key R&D Program of China (2017YFB0307304) ; National Natural Science Foundation of China (21276126, 61673205) ; Project “333” of Jiangsu Province (BRA2016418) ; Six Major Talent Peak Project of Jiangsu Province (XCL-017) ; Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD) ;

Download this article
    References

    [1] MALONE M F, DOHERTY M F. Reactive distillation [J]. Industrial & Engineering Chemistry Research, 2000, 39 (11): 3953–3957.

    [2] GAO X, ZHAO Y, LI H, et al. Review of basic and application investigation of reactive distillation technology for process intensification [J]. CIESC Journal, 2018, 69 (1): 218–238 (in Chinese).

    [3] SUNDMACHER K, QI Z. Reactive Distillation: Status and Future Directions [M]. Weinheim: Wiley-VCH Verlag GmbH & Co. KGa A, 2006.

    [4] AN W Z, LIN Z X, JIANG Y, et al. Design and optimization of an internally heat integrated reactive distillation column for ethylene glycol production [J]. CIESC Journal, 2013, 64 (12): 4634–4640 (in Chinese).

    [5] ZHANG Q R, GUO T, YU C, et al. Design and control of different pressure thermally coupled reactive distillation for amyl acetate synthesis [J]. Chemical Engineering & Processing Process Intensification, 2017, 121: 170–179.

    [6] DING L H, TANG J H, CUI M F, et al. Analysis and comparison of RD and SRC involving consecutive reaction of chlorination of toluene [J]. CIESC Journal, 2013, 64 (9): 3277–3284 (in Chinese).

    [7] WANG Q, YANG C, WANG H, et al. Optimization of process-specific catalytic packing in catalytic distillation process: a multi-scale strategy [J]. Chemical Engineering Science, 2017, 174: 472–486.

    [8] LAI I K, HUNG S B, HUNG W J, et al. Design and control of reactive distillation for ethyl and isopropyl acetates production with azeotropic feeds [J]. Chemical Engineering Science, 2007, 62 (3): 878–898.

    [9] AIOUACHE F, GOTO S. Reactive distillation–pervaporation hybrid column for tert-amyl alcohol etherificatin with ethanol [J]. Chemical Engineering Science, 2003, 58 (12): 2465–2477.

    [10] LUTZE P, GORAK A. Reactive and membrane-assisted distillation: recent developments and perspective [J]. Chemical Engineering Research & Design, 2013, 91 (10): 1978–1997.

    [11] STEINIGEWEG S, GMEHLING J. Transesterification processes by combination of reactive distillation and pervaporation [J]. Chemical Engineering & Processing Process Intensification, 2004, 43 (3): 447–456.

    [12] CHENG X, PAN F, WANG M, et al. Hybrid membranes for pervaporation separations [J]. Journal of Membrane Science, 2017, 541: 329–346.

    [13] ONG Y K, SHI G M, LE N L, et al. Recent membrane development for pervaporation processes [J]. Progress in Polymer Science, 2016, 57: 1–31.

    [14] ZHOU H L, SU Y, YI S L, et al. Effect of acetone and ethanol on pervaporation separation of butanol [J]. CIESC Journal, 2010, 61 (5): 1143–1149 (in Chinese).

    [15] GRIMALDI J, IMBROGNO J, KILDUFF J, et al. A new class of synthetic membranes: organophilic pervaporation brushes for organics recovery [J]. Chemistry of Materials, 2015, 27 (11): 4142–4148.

    [16] RADOSŁAW K, MARTA M, WOJCIECH K, et al. Polyamide-6 based pervaporation membranes for organic–organic separation [J]. Separation & Purification Technology, 2013, 110 (23): 63–73.

    [17] BAKER R W. Research needs in the membrane separation industry: looking back, looking forward [J]. Journal of Membrane Science, 2010, 362 (1/2): 134–136.

    [18] KORELSKIY D, LEPPÄJÄRVI T, ZHOU H, et al. High flux MFI membranes for pervaporation [J]. Journal of Membrane Science, 2013, 427 (1): 381–389.

    [19] ZHANG Y, WANG N, ZHAO C, et al. Co(HCOO)2-based hybrid membranes for the pervaporation separation of aromatic/aliphatic hydrocarbon mixtures [J]. Journal of Membrane Science, 2016, 520: 646–656.

    [20] XU Y M, CHUNG T S. High-performance UiO-66/polyimide mixed matrix membranes for ethanol, isopropanol and n-butanol dehydration via pervaporation [J]. Journal of Membrane Science, 2017, 531: 16–26.

    [21] BUCHALY C, KREIS P, GÓRAK A. Hybrid separation processes—combination of reactive distillation with membrane separation [J]. Chemical Engineering & Processing Process Intensification, 2007, 46 (9): 790–799.

    [22] HARVIANTO G R, AHMAD F, LEE M. A hybrid reactive distillation process with high selectivity pervaporation for butyl acetate production via transesterification [J]. Journal of Membrane Science, 2017, 543: 49–57.

    [23] ARPORNWICHANOP A, KOOMSUP K, ASSABUMRUNGRAT S. Hybrid reactive distillation systems for n-butyl acetate production from dilute acetic acid [J]. Journal of Industrial & Engineering Chemistry, 2008, 14 (6): 796–803.

    [24] LIU K, TONG Z, LIU L, et al. Separation of organic compounds from water by pervaporation in the production of n-butyl acetate via esterification by reactive distillation [J]. Journal of Membrane Science, 2005, 256 (1/2): 193–201.

    [25] HARVIANTO G R, AHMAD F, LEE M. A thermally coupled reactive distillation and pervaporation hybrid process for n-butyl acetate production with enhanced energy efficiency [J]. Chemical Engineering Research & Design, 2017, 124: 98–113.

    [26] HOLTBRUEGGE J, WIERSCHEM M, LUTZE P, et al. Synthesis of dimethyl carbonate and propylene glycol in a membrane-assisted reactive distillation process: pilot-scale experiments, modeling and process analysis [J]. Chemical Engineering & Processing Process Intensification, 2014, 84 (4): 54–70.

    [27] LV B D, LIU G P, DONG X L, et al. Novel reactive distillation–pervaporation coupled process for ethyl acetate production with water removal from reboiler and acetic acid recycle [J]. Industrial & Engineering Chemistry Research, 2012, 51 (23): 8079–8086.

    [28] XIA S S, XU N P, ZHU Y X, et al. A reactive distillation–pervaporation process for production of ethyl acetate: 101402568 A [P]. 2009-04-08 (in Chinese).

    [29] LEE H Y, LI S Y, CHEN C L. Evolutional design and control of the equilibrium-limited ethyl acetate process via reactive distillation–pervaporation hybrid configuration [J]. Industrial & Engineering Chemistry Research, 2016, 55 (32): 8802–8817.

    [30] HANGX G, KWANT G, MAESSEN H, et al. Reaction kinetics of the esterification of ethanol and acetic acid towards ethyl acetate [R]. Technical Report to the European Commission, 2001.

    [31] DOUGLAS J M. Conceptual Design of Chemical Processes [M]. New York: Mc Graw-Hill, 1988: 345–350.

    [32] DING L H, TANG J H, CUI M F, et al. Optimum design and analysis based on independent reaction amount for distillation column with side reactors: production of benzyl chloride [J]. Industrial & Engineering Chemistry Research, 2011, 50 (19): 11143–11152.

    [33] BRUGGEN B V D, LUIS P. Pervaporation as a tool in chemical engineering: a new era? [J]. Current Opinion in Chemical Engineering, 2014, 4: 47–53.

This Article

ISSN:0438-1157

CN: 11-1946/TQ

Vol 69, No. 08, Pages 3469-3478

August 2018

Downloads:0

Share
Article Outline

Knowledge

Abstract

  • Introduction
  • 1 Process
  • 2 Mathematical models
  • 3 Results and discussion
  • 4 Conclusions
  • Symbols
  • References