發(fā)布時間：2018-09-11 20:32

【摘要】：反應(yīng)器是化工生產(chǎn)中實現(xiàn)反應(yīng)過程的關(guān)鍵設(shè)備,反應(yīng)器的過程強(qiáng)化機(jī)理一直是化工界研究的熱點(diǎn)及重點(diǎn)。撞擊流、CIJR)、微/毛細(xì)通道、旋轉(zhuǎn)式等各類反應(yīng)器相繼得到發(fā)展。這些反應(yīng)器的提出,都是基于提高單位時間的傳遞量這一思路,具體則是通過增大流體間接觸面積或增大流體間相對速度實現(xiàn)過程強(qiáng)化。相比于傳統(tǒng)的攪拌反應(yīng)器,這些新型反應(yīng)器的微觀混合性能都有顯著的提高,并被廣泛地應(yīng)用于納米材料制備、萃取過程、吸收、聚合反應(yīng)等方面。然而,上述反應(yīng)器存在設(shè)計加工困難、管路易堵塞、成本高等問題,以至于限制了它們的工業(yè)應(yīng)用。基于上述分析,本文提出了微撞擊流反應(yīng)器(MISR)的概念,并利用商用三通、不銹鋼毛細(xì)管(～1 mm)成功構(gòu)建了微撞擊流反應(yīng)器。MISR反應(yīng)器基于微尺度的設(shè)計理念,同時引入撞擊流技術(shù)優(yōu)勢。該反應(yīng)器采用短粗的放大出口,兩股流體在有限空間內(nèi)發(fā)生強(qiáng)烈撞擊而達(dá)到快速的微觀混合�？梢�,MISR反應(yīng)器具有強(qiáng)化流體混合、降低構(gòu)建難度、減輕管路堵塞的優(yōu)勢。鑒于微撞擊流反應(yīng)器具備良好的微觀混合性能,因此可用于實現(xiàn)液-液相傳質(zhì)以及粉體材料的制備等過程的強(qiáng)化。本文的主要研究內(nèi)容如下：(1)利用商用三通以及不銹鋼毛細(xì)管構(gòu)建MISR反應(yīng)器,通過Iodide-Iodate平行競爭反應(yīng)體系考察MISR反應(yīng)器的微觀混合性能,并采用離集指數(shù)(Xs)進(jìn)行定量分析。研究發(fā)現(xiàn)：增大入口雷諾數(shù)(Rej),Xs隨之減小,當(dāng)Rej3000時,Xs≈0.0003,表明MISR反應(yīng)器具備較高的微觀混合效率；體積流量不一致會導(dǎo)致微觀混合效率變低；流速恒定,入口管徑(di)擴(kuò)大能促進(jìn)微觀混合；而出口管長(L)對微觀混合基本沒有影響,去掉出口管有利于撞擊流的形成。(2)進(jìn)一步借助計算流體力學(xué)(CFD)模擬,可視化研究MISR反應(yīng)器的流體力學(xué)特性和微觀混合-反應(yīng)作用過程。模擬采用標(biāo)準(zhǔn)κ-ε模型,并通過DQMOM-IEM建模方法,探究MISR反應(yīng)器的微觀混合-反應(yīng)作用機(jī)制。當(dāng)Rej3000時,MISR反應(yīng)器中心處形成高湍動能的撞擊核心區(qū),反應(yīng)在極短的時間內(nèi)就進(jìn)行完全；模擬結(jié)果表明,窄長的出口結(jié)構(gòu)不利于MISR反應(yīng)器內(nèi)撞擊流的發(fā)展；模擬經(jīng)實驗數(shù)據(jù)對比驗證為合理的。(3)基于實驗數(shù)據(jù),并結(jié)合團(tuán)聚模型,得到tm與Rej的關(guān)系：當(dāng)Rej1000時,tm=0.84Re-1.07；當(dāng)Rej1000時,tm=27.67Re-1.58；對于MISR反應(yīng)器,tm=0.1～5.0 ms,明顯短于傳統(tǒng)攪拌器的微觀混合時間。利用多種反應(yīng)器的微觀混合/反應(yīng)協(xié)同“操作曲線圖”,并根據(jù)反應(yīng)特征時間,能夠初步篩選反應(yīng)器類型,確定能夠?qū)崿F(xiàn)“微觀混合/反應(yīng)協(xié)同”的操作條件。(4)以液-液兩相流動體系,研究MISR反應(yīng)器兩相流動中的傳質(zhì)特性。結(jié)果表明,水相入口雷諾數(shù)(Reaq)、體積流量比(R)、反應(yīng)器結(jié)構(gòu)以及水相粘度等對反應(yīng)器的總體積傳質(zhì)系數(shù)(KLα)有顯著影響。經(jīng)擬合計算可知,KLα∝(Reαq)1.6,KLα∝(R)-1.2;當(dāng)Reaq=3400,R=1時,MISR反應(yīng)器的總傳質(zhì)系數(shù)約為20 s-1,比傳統(tǒng)的設(shè)備高出2-3個數(shù)量級。應(yīng)用MISR設(shè)備提純蘆�。翰捎贸暋⑽⒉ńM合浸取天然苦蕎蘆丁,經(jīng)正交實驗法,獲得最優(yōu)條件下蘆丁的浸取率為1.7%；通過MISR設(shè)備對浸取液中蘆丁進(jìn)行萃取純化,最優(yōu)條件下蘆丁的萃取率為78.8%。(5)MISR反應(yīng)器應(yīng)用于超細(xì)二氧化錳的制備。實驗結(jié)果表明：增大入口流速,采用攪拌陳化處理,都能提高材料的性能；體積流量不一致會引起產(chǎn)物的比容量降低；最優(yōu)條件下制得球形α-MnO2,粒徑約為120 nm,比表面積～200 m2·g-1,最高放電比容量達(dá)211 F·g-1,循環(huán)1000次后衰減18%。利用MISR反應(yīng)器對二氧化錳進(jìn)行摻鐵改性：以FeCl3為鐵源,Mn:Fe=20:1的條件下,產(chǎn)物比容量為200 F·g-1,經(jīng)1000次循環(huán)后衰減7%,穩(wěn)定性較未摻鐵的材料(33%)有顯著提升。
[Abstract]:Reactor is the key equipment to realize the reaction process in chemical production. The mechanism of process intensification has always been the focus of chemical research. Impinging stream, CIJR, micro/capillary channel, rotating reactor and other types of reactors have been developed one after another. Compared with conventional stirred reactors, these new reactors have significantly improved micro-mixing performance and are widely used in the preparation of nanomaterials, extraction processes, absorption, polymerization and other aspects. Based on the above analysis, the concept of micro impinging stream reactor (MISR) is proposed, and a micro impinging stream reactor (MICR) is successfully constructed using commercial tee and stainless steel capillary (~1 mm). The MISR reactor is based on the design concept of micro-scale. This reactor adopts a short and thick enlarged outlet, and the two fluids collide strongly in a limited space to achieve rapid micro-mixing. It can be seen that the MISR reactor has the advantages of strengthening fluid mixing, reducing the difficulty of construction, and reducing pipeline blockage. The main research contents of this paper are as follows: (1) The MISR reactor was constructed by commercial tee and stainless steel capillary. The micro-mixing performance of the MISR reactor was investigated by Iodide-Iodate parallel competitive reaction system, and the separation index (Xs) was used. Quantitative analysis was carried out. It was found that with the increase of Rej, Xs decreases. When Rej 3000, Xs_0.0003 indicates that MISR reactor has a high micro-mixing efficiency; inconsistent volume flow leads to low micro-mixing efficiency; constant flow rate, enlarged inlet diameter (di) can promote micro-mixing; and outlet pipe length (L) is relatively small. (2) With the help of computational fluid dynamics (CFD), the hydrodynamic characteristics and micro-mixing-reaction process of MISR reactor were visualized. The standard k-e model was used to simulate the micro-mixing-reaction process of MISR reactor, and the DQMOM-IEM modeling method was used to explore the micro-mixing-reaction process of MISR reactor. Reaction mechanism. When Rej3000, a high turbulent kinetic energy impinging core zone was formed in the center of MISR reactor, and the reaction was completed in a very short time. The simulation results show that the narrow and long exit structure is not conducive to the development of impinging stream in MISR reactor. The simulation results are verified to be reasonable by comparing the experimental data. (3) Based on the experimental data, the reaction is completed. The relationship between TM and Rej was obtained by agglomeration model: when Rej 1000, TM = 0.84 Re-1.07; when Rej 1000, TM = 27.67 Re-1.58; for MISR reactor, TM = 0.1-5.0 ms, obviously shorter than the micro-mixing time of traditional agitator. (4) Mass transfer characteristics in the two-phase flow of a MISR reactor were studied in a liquid-liquid two-phase flow system. The results showed that the total mass transfer of the reactor was affected by the Reynolds number at the inlet of the water phase (Reaq), the volume flow ratio (R), the structure of the reactor and the viscosity of the water phase. The results show that the total mass transfer coefficient of MISR reactor is about 20 S-1 when Reaq = 3400 and R = 1, which is 2-3 orders of magnitude higher than that of traditional equipment. The extraction rate of Rutin in the leaching solution was 78.8%. (5) MISR reactor was applied to the preparation of ultrafine manganese dioxide. The results showed that the performance of the material could be improved by increasing the inlet flow rate and agitating and aging treatment. Under the optimum conditions, spherical alpha-MnO2 with a particle size of 120 nm, a specific surface area of 200 m2.g-1, a maximum discharge specific capacity of 211 F.g-1 and a decay of 18% after 1000 cycles were prepared. 00 F? G-1, after 1000 cycles of attenuation 7%, and stability than non iron doped material (33%) has significantly improved.
【學(xué)位授予單位】：北京化工大學(xué)
【學(xué)位級別】：博士
【學(xué)位授予年份】：2015
【分類號】：TQ052

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