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膜微反應(yīng)器中流動(dòng)與傳質(zhì)性能研究及其應(yīng)用

發(fā)布時(shí)間:2018-05-11 08:29

  本文選題:膜微反應(yīng)器 + 微通道; 參考:《北京化工大學(xué)》2015年博士論文


【摘要】:化工過(guò)程強(qiáng)化技術(shù)是在不改變已定生產(chǎn)任務(wù)的同時(shí),通過(guò)縮小設(shè)備體積,簡(jiǎn)化生產(chǎn)工藝,壓縮設(shè)備數(shù)量,使整體產(chǎn)線布局更加緊湊合理,顯著降低能耗、廢料和副產(chǎn)品產(chǎn)出。發(fā)展新型反應(yīng)分離耦合技術(shù)與裝置對(duì)化工反應(yīng)過(guò)程強(qiáng)化具有重要的理論意義和應(yīng)用價(jià)值。微化工系統(tǒng)的出現(xiàn)為綠色、安全、高效的完成反應(yīng)過(guò)程提供了新的技術(shù)和方法,而膜反應(yīng)技術(shù)通過(guò)反應(yīng)與分離耦合實(shí)現(xiàn)了生產(chǎn)過(guò)程的有效強(qiáng)化。論文將微流控技術(shù)與膜分離技術(shù)結(jié)合,設(shè)計(jì)發(fā)展新型膜微反應(yīng)器,從而實(shí)現(xiàn)反應(yīng)-分離耦合過(guò)程的強(qiáng)化。但是,作為一個(gè)新的研究方向,目前關(guān)于膜微反應(yīng)器的理論研究非常少,要實(shí)現(xiàn)反應(yīng)與分離耦合過(guò)程的強(qiáng)化,需要對(duì)膜微反應(yīng)器內(nèi)流體流動(dòng)、傳質(zhì)及膜壁面?zhèn)髻|(zhì)性能有深入的研究。本論文首先以矩形微通道為液相流動(dòng)規(guī)律研究平臺(tái),探討了微尺度下流動(dòng)基本規(guī)律。通過(guò)可視化實(shí)驗(yàn)與計(jì)算流體力學(xué)模擬,分析了流體與通道壁面浸潤(rùn)性能對(duì)液相流動(dòng)的影響。通過(guò)分析不同流型時(shí)微通道內(nèi)擠壓力、剪切力和界面張力的作用關(guān)系,指出了用連續(xù)相流速表示剪切力大小,使用兩相流量作為劃分流型的主要依據(jù),實(shí)現(xiàn)了多種流型(層流、液柱分散流、液滴分散流等)問(wèn)的可控轉(zhuǎn)換。對(duì)不同流型時(shí)的速度場(chǎng)進(jìn)行了分析,指出不同流場(chǎng)下主導(dǎo)作用力的區(qū)別。為膜微反應(yīng)器中流體流動(dòng)規(guī)律的研究提供了理論基礎(chǔ)。其次,利用滲透汽化膜微反應(yīng)器考察了不同操作條件下膜分離性能。系統(tǒng)研究了不同料液溫度、水含量和流速時(shí),膜微反應(yīng)器對(duì)正丁醇/水體系的分離性能。根據(jù)溶解-擴(kuò)散機(jī)理,采用串聯(lián)阻力模型,建立了滲透汽化傳質(zhì)半經(jīng)驗(yàn)?zāi)P。為膜微反?yīng)器應(yīng)用于反應(yīng)-分離耦合過(guò)程提供了理論依據(jù)。再者,基于微通道中流體流動(dòng)基礎(chǔ)理論,建立了膜微反應(yīng)器中流動(dòng)方程,并利用有限傅立葉變換求解此方程,通過(guò)滲透汽化脫水過(guò)程,評(píng)價(jià)模型的使用。在流動(dòng)模型的基礎(chǔ)上,建立了膜微反應(yīng)器中二組元對(duì)流擴(kuò)散模型,通過(guò)模擬計(jì)算得到出口截面水濃度,并與實(shí)驗(yàn)結(jié)果相比較。豐富了微尺度下流體流動(dòng)的基本理論。最后,在膜微反應(yīng)器內(nèi)流動(dòng)與傳質(zhì)性能研究的基礎(chǔ)上,以酯化反應(yīng)為例,分析了催化膜微反應(yīng)器對(duì)滲透汽化-反應(yīng)耦合過(guò)程的強(qiáng)化作用。在相同的反應(yīng)條件下,膜微反應(yīng)器內(nèi)反應(yīng)轉(zhuǎn)化率較常規(guī)尺寸膜反應(yīng)器中有很大提高,并且在膜微反應(yīng)器中可有效減緩催化劑失活。
[Abstract]:Chemical process strengthening technology is to reduce the volume of equipment, simplify the production process, compress the number of equipment, make the overall production line layout more compact and reasonable, significantly reduce energy consumption, waste and by-product output. The development of new reaction separation coupling technology and equipment has important theoretical significance and application value for chemical reaction process strengthening. The emergence of micro-chemical systems provides a new technique and method for green, safe and efficient completion of the reaction process, while the membrane reaction technology can effectively strengthen the production process through the coupling of reaction and separation. In this paper, a new membrane microreactor is designed and developed by combining microfluidic technology with membrane separation technology, so that the coupling process between reaction and separation can be strengthened. However, as a new research direction, there is very little theoretical research on membrane microreactor. In order to enhance the coupling process of reaction and separation, fluid flow in membrane microreactor is needed. Mass transfer and film wall mass transfer properties have been studied in depth. In this paper, rectangular microchannels are first used as the platform for the study of liquid flow law, and the basic law of flow at microscale is discussed. The effects of fluid and channel wall wettability on liquid phase flow were analyzed by visual experiment and computational fluid dynamics simulation. By analyzing the relationship between extrusion force, shear force and interfacial tension in microchannel with different flow patterns, it is pointed out that the shear force is represented by the velocity of continuous phase and the flow rate of two phases is used as the main basis for classifying flow patterns, and various flow patterns (laminar flow) are realized. Column dispersion, droplet dispersion, etc. The velocity field of different flow patterns is analyzed and the difference of dominant forces under different flow patterns is pointed out. It provides a theoretical basis for the study of fluid flow in membrane microreactor. Secondly, membrane separation performance under different operating conditions was investigated by pervaporation membrane microreactor. The separation performance of n-butanol / water system by membrane microreactor with different feed temperature, water content and flow rate was studied systematically. According to the mechanism of solution-diffusion, a semi-empirical model of osmotic vaporization mass transfer was established by using the series resistance model. It provides a theoretical basis for the application of membrane microreactor in the reaction-separation coupling process. Furthermore, based on the basic theory of fluid flow in microchannels, the flow equation in membrane microreactor is established, and the finite Fourier transform is used to solve the equation. The application of the model is evaluated through the process of pervaporation and dehydration. Based on the flow model, a two-component convection-diffusion model in a membrane microreactor was established. The water concentration at the outlet section was calculated by simulation, and the results were compared with the experimental results. It enriches the basic theory of fluid flow in microscale. Finally, based on the study of flow and mass transfer in membrane microreactor, the enhancement effect of catalytic membrane microreactor on the coupling process of pervaporation and reaction was analyzed by taking esterification as an example. Under the same reaction conditions, the conversion rate in the membrane microreactor is much higher than that in the conventional membrane reactor, and the deactivation of the catalyst can be effectively slowed down in the membrane microreactor.
【學(xué)位授予單位】:北京化工大學(xué)
【學(xué)位級(jí)別】:博士
【學(xué)位授予年份】:2015
【分類(lèi)號(hào)】:TQ052

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