本文選題：氣液反應(yīng)動(dòng)力學(xué) + 液體進(jìn)樣裝置　； 參考：《山東大學(xué)》2015年碩士論文

【摘要】：氣液反應(yīng)機(jī)理的研究及反應(yīng)動(dòng)力學(xué)參數(shù)的求算是材料、環(huán)境、化工、化學(xué)等領(lǐng)域研究開發(fā)的基礎(chǔ)。本文自主研發(fā)了高粘度液體原料快速進(jìn)樣系統(tǒng),并將其同微型流化床氣固反應(yīng)一體機(jī)的結(jié)構(gòu)和控制系統(tǒng)進(jìn)行連接與匹配,形成適用于液體原料的微型流化床反應(yīng)分析儀(MFBRA-L:Micro Fluidized Bed Reaction Analyzer for Liquid Reactants)。該分析儀可彌補(bǔ)在液體原料等溫微分反應(yīng)方面現(xiàn)有分析手段的不足,具有廣泛的應(yīng)用前景。本文將MFBRA-L的設(shè)計(jì)原理、研究現(xiàn)狀及其技術(shù)要點(diǎn)進(jìn)行了闡述。然后展示了MFBRA-L在液體原料熱解、燃燒、催化裂解三種典型氣液反應(yīng)的應(yīng)用特性。首先,為了測(cè)定設(shè)定溫度下的液體原料反應(yīng)機(jī)理,所設(shè)計(jì)的MFBRA-L主要包括氣體供給系統(tǒng)、液體原料進(jìn)樣系統(tǒng)、流化床反應(yīng)系統(tǒng)以及數(shù)據(jù)采集與分析系統(tǒng)四部分。通過液體原料進(jìn)樣系統(tǒng)將原料快速送入到流化床反應(yīng)系統(tǒng),在氣體供給系統(tǒng)提供的流化氣體的作用下,氣體產(chǎn)物進(jìn)入過程質(zhì)譜,從而實(shí)現(xiàn)在線監(jiān)測(cè)分析及數(shù)據(jù)采集。其中的液體原料進(jìn)樣系統(tǒng)主要采用氣壓缸帶動(dòng)注射泵實(shí)現(xiàn)液體原料的快速進(jìn)樣,整個(gè)過程可以實(shí)現(xiàn)自動(dòng)化控制。其次,利用MFBRA-L研究了苯類焦油模化物苯、甲苯和二甲苯在氬氣氣氛中的熱解反應(yīng)動(dòng)力學(xué)特性。研究結(jié)果表明：應(yīng)用MFBRA-L測(cè)定的三種反應(yīng)物在反應(yīng)溫度區(qū)間(650～850℃)的反應(yīng)時(shí)間尺度均小于10s。苯、甲苯和二甲苯裂解反應(yīng)生成H2或CH4的表觀活化能均依次減小。對(duì)于三種不同的反應(yīng)物,生成H2的表觀活化能均大于生成CH4的表觀活化能。測(cè)試的氣體釋放順序與反應(yīng)動(dòng)力學(xué)參數(shù)證實(shí)了各氣體生成難易程度存在差異。再次,應(yīng)用MFBRA-L研究了甲苯在不同N2/02配比氣氛下的燃燒動(dòng)力學(xué)特性。研究結(jié)果表明：氧氣濃度變化對(duì)甲苯的熱解反應(yīng)速率以及反應(yīng)動(dòng)力學(xué)參數(shù)具有較大影響。氧氣濃度越高,反應(yīng)生成H2、CH4和C02的表觀活化能均越低；相同氧氣濃度下,甲苯生成H2、CH4和CO2時(shí)的表觀活化能均依次減小。說(shuō)明氧氣濃度的增高能夠促進(jìn)反應(yīng)的進(jìn)行,反應(yīng)更加容易。最后,本文以苯酚為熱解反應(yīng)原料,以高純氬氣作為流化氣體,在MFBRA-L上分別進(jìn)行苯酚裂解反應(yīng)和催化裂解反應(yīng),研究結(jié)果表明：催化劑白云石以及氧化鈣能夠明顯影響苯酚的裂解反應(yīng),但是對(duì)不同產(chǎn)物的影響程度有所不同。其中催化劑對(duì)產(chǎn)物H2的影響最為明顯,對(duì)C02的影響次之,對(duì)CO和CH4影響最小。在700℃時(shí),相較于不使用催化劑,使用白云石和氧化鈣分別能使H2的產(chǎn)量提高約80倍和20倍,能使總氣體產(chǎn)量提高約4.9倍和1.6倍。苯酚裂解生成H2和CO的表觀活化能平均值分別為73.94 kJ/mol和83.77 kJ/mol。白云石催化裂解苯酚生成H2和CO的表觀活化能平均值分別為38.66 kJ/mol和47.37 kJ/mol,氧化鈣催化裂解苯酚生成H2和CO的表觀活化能平均值分別為44.26 kJ/mol和52.77 kJ/mol。催化劑白云石和氧化鈣的使用能夠明顯降低苯酚裂解反應(yīng)的活化能,加快反應(yīng)速率,具有良好的催化效果。
[Abstract]:The research on the mechanism of gas-liquid reaction and the calculation of the kinetic parameters of the reaction are the basis for the research and development of materials, environment, chemical and chemical fields. This paper independently developed a rapid sampling system for high viscosity liquid materials, and connected it with the structure and control system of a micro fluidized bed gas solid reaction machine to form a liquid suitable for liquid. The micro fluidized bed reaction analyzer (MFBRA-L:Micro Fluidized Bed Reaction Analyzer for Liquid Reactants). The analyzer can make up for the shortcomings of the existing analytical means in the isothermal differential reaction of liquid materials, and has a wide application prospect. This paper expounds the design principle of MFBRA-L, the research status and technical points of this paper. The application characteristics of the three typical gas-liquid reactions of MFBRA-L in the pyrolysis, combustion and catalytic cracking of liquid materials are presented. First, in order to determine the reaction mechanism of liquid raw materials at set temperatures, the designed MFBRA-L mainly includes the gas supply system, the liquid feed system, the fluidized bed reaction system and the data acquisition and analysis system. The four part, through the liquid raw material feeding system, quickly sent the raw materials into the fluidized bed reaction system. Under the action of the fluidizing gas provided by the gas supply system, the gas products entered the process mass spectrometry, thus the on-line monitoring analysis and data collection were realized. The liquid raw material injection system mainly used the pressure cylinder to drive the injection pump to realize the liquid. Automatic control of the whole process can be achieved in the whole process. Secondly, the kinetic characteristics of the pyrolysis reaction of benzene, toluene and xylene in argon atmosphere are studied by MFBRA-L. The results show that the reaction time scale of the three reactants measured by MFBRA-L in the reaction temperature range (650~850 degrees C) The apparent activation energy of H2 or CH4, which is less than 10s. benzene, and toluene and xylene cracking reaction, decreases in turn. For the three different kinds of reactants, the apparent activation energy of the formation of H2 is greater than the apparent activation energy of the formation of CH4. The gas release sequence and the kinetic parameters of the test confirm the difference in the difficulty degree of each gas generation. The kinetic characteristics of Toluene Combustion in different N2/02 ratio atmosphere were studied by MFBRA-L. The results showed that the change of oxygen concentration had great influence on the pyrolysis rate and kinetic parameters of toluene. The higher the oxygen concentration, the reaction generated H2, the apparent activation energy of CH4 and C02 was lower, and the toluene was born under the same oxygen concentration. The apparent activation energy of H2, CH4 and CO2 decreased in turn. It shows that the increase of oxygen concentration can promote the reaction and the reaction is easier. Finally, the phenol is used as the raw material for the pyrolysis reaction and the high pure argon is used as the fluidizing gas. The reaction of the reaction and the catalytic cracking of the phenol pyrolysis is carried out on the MFBRA-L. The results show that the catalyst is used as a catalyst. Dolomite and calcium oxide can obviously affect the cracking reaction of phenol, but the influence on different products is different. The effect of catalyst on H2 is the most obvious, the effect on C02 is the second, and the smallest effect on CO and CH4. At 700 C, the use of dolomite and calcium oxide can make the production of H2, respectively, compared with the use of the dolomite and calcium oxide. The increase of total gas production by about 80 times and 20 times increases the total gas production by about 4.9 times and 1.6 times. The apparent activation energy of the apparent activation energy of H2 and CO by phenol cracking is 73.94 kJ/mol and 83.77 kJ/mol. in the catalytic cracking of phenol to produce H2 and CO, the average value of the activation energy is 38.66 kJ/mol and 47.37 kJ/mol, and the calcium oxide catalytic cracking phenol produces H2, respectively. The average value of apparent activation energy of CO and CO, respectively, is 44.26 kJ/mol and 52.77 kJ/mol. catalyst dolomite and calcium oxide can obviously reduce the activation energy of the phenol pyrolysis reaction, accelerate the reaction rate and have good catalytic effect.
【學(xué)位授予單位】：山東大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：TQ051.13

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