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Exploring Distillation-Pervaporation Hybrid Process in a Single Column Using Hollow fiber Pervaporation Composite Membranes As Structured Packing

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Exploring Distillation-Pervaporation Hybrid Process in a Single Column Using Hollow fiber Pervaporation Composite Membranes As Structured Packing Materials Express 2158-5849/2020/10/701/009 Copyright © 2020 by American Scientific Publishers All rights reserved. doi:10.1166/mex.2020.1680 Printed in the United States of America www.aspbs.com/mex Exploring distillation-pervaporation hybrid process in a single column using hollow fiber pervaporation composite membranes as structured packing Liwei Zhuang, Qingyuan Cao, Fei Liang, Yichao Hu, Weite Su, Xin Wen, Xiao-Hua Ma∗, and Zhen-Liang Xu State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China ABSTRACT Article This study developed a novel strategy for azeotrope separation such as ethanol-water binary system. Distillation-pervaporation hybridIP: 192.168.39.211 process was On: employed Fri, 01 Oct by 2021 using 04:07:40 hollow fiber pervaporation composite Copyright: American Scientific Publishers membranes as structured packing in a singleDelivered hybrid by column Ingenta rather than using pervaporation as an externally connected unit of the distillation column. The separating limitation of azeotrope challenged in conventional dis- tillation could be readily overcome by continually removing water from the hybrid system via pervaporation. The competition between distillation and pervaporation has been found to be cause of unexpected concentra- tion distribution in the hybrid column. The mass flux of mixture decreased with time whereas the selectivity of water to ethanol first increased then decreased with time. Analysis of this system illustrated that the increase in heating power and membrane area shortened time for obtaining certain content of ethanol in the mixture. However, faster decline in mass flux occurred due to an increase in the removal rate of water. With respect to its simplicity, efficiency and broad applicability, this hybrid process is expected to provide a benchmark for the enhancement of distillation-pervaporation process by hollow fiber membrane packing. Keywords: Pervaporation, Distillation, Hybrid Column, Hollow Fiber Structured Packing, Azeotrope Separation. 1. INTRODUCTION powerful weapon in combating global warming and a key Process integration is now a widely accepted technique for technology to realize green processes. designing sustainable and green chemical processes [1]. Currently, distillation and related operations are still the It refers to “complex technologies that replace large, most commonly employed separation processes, involved expensive, energy-intensive equipment or processes with in more than 95% of industrial applications in the chemical smaller, less costly, more efficient plants, or plants that industries [4, 5]. However, the separation of a large number combine multiple operations into a single apparatus or into of industrial solvent mixtures containing azeotropes which fewer devices” [2], to make the factory layout more com- cannot be separated through traditional distillation due to pact and reasonable, with lower unit consumption, less the identical composition in liquid and vapour phases. waste and byproducts, and eventually to improve produc- In addition, distillation is an energy intensive technology, tion efficiency, reduce production cost, improve security which is a considerable source of pollutants and green- and reduce environmental pollution [3]. It is therefore a house gases or a high consumption of auxiliary agents such as entrainer [6, 7]. Therefore, a drastic development in the field of azeotrope separation is of great significance and ∗Author to whom correspondence should be addressed. extremely urgent [8]. Mater. Express, Vol. 10, No. 5, 2020 701 Materials Express Exploring distillation-pervaporation hybrid process in a single column Zhuang et al. Pervaporation is a membrane separation process in side of the hollow fibers without direct contact. The mass which a certain component of liquid mixture preferentially transfer is merely driven by the concentration gradient permeates through a dense membrane/porous ceramic without the presence of two-phase mixing. Thanks to the membrane and evaporates downstream [9]. The selectiv- operation, the hydrodynamic problems such as flooding, ity of pervaporation is governed by the transport rate of loading, weeping, foaming that are frequently found in the molecules through the membrane due to the differ- conventional devices disappear, presenting good chemi- ence in solubility and diffusivity among the components cal/thermal stability and high separation efficiency. Ma and rather than relative volatility. It is therefore one of the most coworkers employed a new process [32]. They used hol- potential technologies for azeotropic separations and the low fiber membrane as structured packing in a distillation like [10–12]. In addition, pervaporation is considered as column, in which, both vapour and liquid flow on the feed an energy saving process for separation [13–15]. side of the hollow fiber membranes. The mass transfer then Distillation integrated with pervaporation can potentially takes place on the feed side of the membranes with mixing exploit and improve the performance that both technology of the two phases. Compared with conventional packing will achieve separately, while overcoming the disadvan- such as Raschig ring, Berl saddle, Mellapark (250Y) and tages of both [10, 16]. The first reported work regarding so on, a better performance is observed and the height of a distillation column integrated with membranes for per- transfer unit can be reduced to 3.6 cm (with current vapour vaporation or vapour permeation in the same column can velocity 39.4 cm/s) and also can be operated above the be seen in the patent by Fontalvo et al. [17]. A series of flooding line. further studies have been conducted, which significantly Better separating performance could be expected promote the understanding and application of distillation- through hybrid distillation and pervaporation together pervaporation hybrid system [5, 16, 18–22]. A traditional since the azeotrope limitation could be broken by pervapo- distillation-pervaporation hybrid system is comprised of ration. In addition, there is no need for inter-stage heating a distillation column and an externally connected perva- because the energy required for pervaporation is supplied poration module, either removing a specific component by the condensation of the vapour, and the hybrid pro- from a side stream of the distillation column or used cess provides a convenient geometry since it is relatively as a final treatment stage [12,IP: 16]. 192.168.39.211 However, a tempera- On: Fri, 01compact Oct 2021 and 04:07:40 allows good vapour and liquid distributions. ture drop along the membrane existsCopyright: as the components American ScientificTherefore, Publishers in the present work, hollow fiber pervapora- permeate and evaporate through the membrane,Delivered which by Ingentation composite membranes with a dense separation layer leads to the demand for the inter-stage heat exchangers on the outside surface were used as structured packing to between the consecutive pervaporation modules where the combine distillation and pervaporation together in a single Article retentate flows between stages in liquid phase [13, 23]. column. The performances of the pervaporation-distillation Fontalvo et al. found that a retentate stream composed hybrid process were analyzed and it was expected that of liquid and vapour could cause significant decrease in this analysis would provide guidance for the research on requirements of membrane area (about 20–40%) and no distillation-pervaporation hybrid process. inter-stage heat exchangers would be needed [24, 25]. This special operation of liquid-vapour feed enables the 2. EXPERIMENTAL DETAILS reduction in capital cost and mitigation of the effects 2.1. Materials and Hollow Fiber Pervaporation of concentration/temperature polarization. Meanwhile, the Membrane Fabrication vapour phase has intensified the heat and mass transfer by All the reagents were purchased from Sinopharm Group supplying heat through condensation and promoting two- Co. Ltd., Shanghai, China, and used without further purifi- phase instability. Therefore, a proper configuration for a cation. Deionized water was used throughout the work. distillation-pervaporation hybrid system will be of great The hollow fiber pervaporation membranes could be importance. purchased from Sulzer or any other supplier, whereas To this end, a novel coupling method was employed the ones used in the current work were home-made and in the present work: hollow fiber membranes were used reported previously [33]. Firstly, polyacrylonitrile (PAN) as structured packing as well as the pervaporation mem- hollow fiber ultrafiltration membranes were fabricated via branes to combine distillation and pervaporation processes nonsolvent induced phase inversion (mass fraction ratio: together in a single column. In feed side of membrane, PAN/polyvinylpyrrolidone/dimethylacetamide = 15/4/81). vapour and liquid flow in counter-current mode as the two Secondly, PAN hollow fiber membranes were coated by phases in distillation, and in the permeate side, the per- 8.0 wt% polyvinyl alcohol aqueous solution for 30 sec- meate is collected to achieve the pervaporation process. onds and hanged vertically singly to dry at room temper- Cussler et al. [26–28], and many other researchers [29–31], ature. Thirdly, the coated PAN hollow fiber membranes have adopted hollow fiber membranes as structured pack- were crosslinked by glutaraldehyde crosslinking solution = ing in membrane
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