本文選題：甲醇 + 2-甲基-1-丁醇�。� 參考：《中國(guó)科學(xué)技術(shù)大學(xué)》2016年碩士論文

【摘要】：能源是國(guó)民經(jīng)濟(jì)的動(dòng)力和命脈�；剂系娜紵峁┝巳�85%和我國(guó)近90%的一次能源需求�，F(xiàn)如今化石燃料的急劇消耗不僅帶來(lái)了前所未有的能源危機(jī),還釀成了環(huán)境污染的惡果,時(shí)刻威脅著環(huán)境安全和人類(lèi)健康。生物醇類(lèi),可以用作汽油的添加劑或者替代燃料,一方面可以減緩人類(lèi)對(duì)化石燃料的過(guò)分依賴(lài),另一方面醇類(lèi)燃料中的C02排放和吸收構(gòu)成自然界碳循環(huán),可實(shí)現(xiàn)C02近零排放。目前,國(guó)際上對(duì)生物醇類(lèi)的研究涵蓋C1-C8的醇類(lèi)。其中甲醇是最簡(jiǎn)單的醇類(lèi),作為汽油添加劑,可以有效增加燃料的辛烷值,提高抗爆性,進(jìn)而改善引擎表現(xiàn),提高引擎效率。此外,甲醇還是研究其它醇類(lèi)的模型燃料,因此,對(duì)甲醇燃料燃燒反應(yīng)動(dòng)力學(xué)進(jìn)行深入研究具有重要意義。作為長(zhǎng)鏈醇類(lèi)的代表之一,2-甲基-1-丁醇(活性戊醇)是一種含有5個(gè)碳原子的醇類(lèi),相比分子量較小的甲醇,它表現(xiàn)出諸多明顯的優(yōu)勢(shì),比如：能量密度大,具有較低蒸汽壓,疏水性強(qiáng),可與碳?xì)浠衔锖芎没ト艿?因此2-甲基-1-丁醇非常適合作為運(yùn)輸燃料,是不久的將來(lái)能作為實(shí)際輸運(yùn)燃料中添加劑或替代燃料的熱門(mén)生物燃料之一。因此,本論文選擇短鏈的甲醇和長(zhǎng)鏈的2-甲基-1-丁醇作為研究對(duì)象,深入分析醇類(lèi)燃料熱解和燃燒的基本規(guī)律,一方面優(yōu)化甲醇燃燒模型,使其作為研究醇類(lèi)燃燒的基本模型；另一方面,以2-甲基-1-丁醇為代表,探索大分子醇類(lèi)燃料燃燒過(guò)程中燃料的分解規(guī)律。本文的研究?jī)?nèi)容主要包括實(shí)驗(yàn)和模型研究?jī)纱蠓矫?對(duì)甲醇開(kāi)展了火焰?zhèn)鞑ニ俣鹊臏y(cè)量和層流預(yù)混火焰的診斷實(shí)驗(yàn),兼顧宏觀燃燒參數(shù)和微觀反應(yīng)動(dòng)力學(xué)數(shù)據(jù)的采集。甲醇的層流火焰?zhèn)鞑ニ俣葴y(cè)量利用了本組的燃燒彈實(shí)驗(yàn)平臺(tái),未燃預(yù)混燃?xì)鉁囟葹?23 K,實(shí)驗(yàn)測(cè)量的燃燒壓力條件為1-10 atm。甲醇的層流預(yù)混火焰實(shí)驗(yàn)借助本組最新研制出的層流預(yù)混火焰實(shí)驗(yàn)平臺(tái),并利用超聲分子束取樣結(jié)合同步輻射真空紫外光電離質(zhì)譜技術(shù)(SVUV-PIMS)展開(kāi),測(cè)量了甲醇燃燒過(guò)程中穩(wěn)定產(chǎn)物以及活潑中間體的濃度信息,實(shí)驗(yàn)壓力30Torr,當(dāng)量1.0。本工作對(duì)活性戊醇開(kāi)展了變壓力的流動(dòng)管熱解研究,重點(diǎn)測(cè)量其分解過(guò)程中初級(jí)產(chǎn)物的濃度信息。2-甲基-1-丁醇的變壓力流動(dòng)管熱解實(shí)驗(yàn)也使用了超聲分子束取樣結(jié)合同步輻射真空紫外光電離質(zhì)譜技術(shù)(SVUV-PIMS),實(shí)驗(yàn)壓力條件30和760 Torr,溫度范圍在750-1400 K。此外,基于對(duì)前人實(shí)驗(yàn)、理論計(jì)算和模型研究數(shù)據(jù)的全面收集,本文構(gòu)建了甲醇的燃燒反應(yīng)動(dòng)力學(xué)模型,并利用CHEMKIN-PRO軟件對(duì)文獻(xiàn)和本文實(shí)驗(yàn)數(shù)據(jù)進(jìn)行了驗(yàn)證,發(fā)展并優(yōu)化了一個(gè)能夠在寬廣實(shí)驗(yàn)工況下預(yù)測(cè)良好的甲醇模型。同時(shí),發(fā)展了2-甲基-1-丁醇的熱解模型,并與本課題組之前研究的丁醇異構(gòu)體的熱解進(jìn)行詳細(xì)對(duì)比,探討了碳鏈增長(zhǎng)和支鏈結(jié)構(gòu)對(duì)醇類(lèi)燃料熱解的影響。具體研究成果如下：首先,通過(guò)燃燒彈實(shí)驗(yàn),測(cè)量了甲醇1-10 atm下,當(dāng)量比為0.7-2.1的火焰?zhèn)鞑ニ俣�。通過(guò)分析高壓和極富燃條件下的反應(yīng)機(jī)制發(fā)現(xiàn),HO2自由基是高壓和富燃條件下火焰?zhèn)鞑ミ^(guò)程中的主要自由基,與它相關(guān)的反應(yīng)在該條件下對(duì)甲醇火焰?zhèn)鞑ニ俣鹊念A(yù)測(cè)非常敏感。本工作更新了氫氣機(jī)理中涉及H02轉(zhuǎn)化的反應(yīng)速率常數(shù),以及甲醛和甲醇子機(jī)理中H02的生成和消耗反應(yīng)速率,這些更新會(huì)對(duì)火焰?zhèn)鞑ンw系自由基池的預(yù)測(cè)帶來(lái)較大影響,同時(shí)大大改善了前人模型對(duì)高壓和富燃條件下火焰?zhèn)鞑ニ俣鹊念A(yù)測(cè)。其次,利用SVUV-PIMS方法鑒別了前人無(wú)法區(qū)分的羥甲基自由基(CH2OH)和甲氧基自由基(CH30),并對(duì)羥甲基自由基CH2OH進(jìn)行定量測(cè)量。基于CH2OH的摩爾分?jǐn)?shù)信息,以及實(shí)驗(yàn)測(cè)得的其它C1產(chǎn)物進(jìn)行模型研究,發(fā)現(xiàn)前人過(guò)高估計(jì)了由羥甲基自由基生成甲醛的路徑,即CH2OH+O2=CH2O+HO2的反應(yīng)速率在高溫下被高估。此外,通過(guò)本工作的實(shí)驗(yàn)結(jié)果驗(yàn)證,發(fā)現(xiàn)前人的甲醇模型中C2物種來(lái)自甲基復(fù)合,效率很低,因此,本工作探討了羥甲基自由基CH2OH復(fù)合生成C2物種的路徑,這些反應(yīng)路徑的加入大大改善了模型對(duì)C2物種的預(yù)測(cè)情況。最后,利用SVUV-PIMS方法,對(duì)2-甲基-1-丁醇的熱解中間體進(jìn)行全面探測(cè),發(fā)展并驗(yàn)證了一個(gè)2-甲基-1-丁醇的熱解模型。通過(guò)對(duì)比丁醇異構(gòu)體熱解規(guī)律,我們發(fā)現(xiàn)2-甲基-1-丁醇的熱解機(jī)制與異丁醇的熱解機(jī)制相近,而與正丁醇相差很大。兩種支鏈醇在熱解中都表現(xiàn)出單分子解離反應(yīng)的貢獻(xiàn)比H提取反應(yīng)的貢獻(xiàn)要小很多的特點(diǎn)。
[Abstract]:Energy is the driving force and lifeblood of the national economy. The burning of fossil fuels provides 85% of the world and nearly 90% of our country's energy demand. Today, the rapid consumption of fossil fuels has not only brought unprecedented energy crises, but also resulted in environmental pollution, threatening environmental safety and human health. Biological alcohols can be used as a result. Gasoline additives or alternative fuels, on the one hand, can slow down human dependence on fossil fuels. On the other hand, the C02 emission and absorption in the alcohols fuels the natural carbon cycle, which can achieve the near zero emission of C02. At present, the international study of biological alcohols covers the alcohols of C1-C8. Oil additives can effectively increase the octane number of fuel, improve the anti explosion, improve engine performance and improve engine efficiency. In addition, methanol is still a model fuel for other alcohols. Therefore, it is important to study the combustion kinetics of methanol fuel. As one of the representative of long chain alcohols, 2- methyl -1- butanol (Live) Amyl alcohol is a kind of alcohol containing 5 carbon atoms. Compared with methanol with smaller molecular weight, it has many obvious advantages, such as high energy density, low vapor pressure, strong hydrophobicity, and good solubility with hydrocarbons. Therefore, 2- methyl -1- butanol is very suitable as a transport fuel, and it can be used as a practical future in the near future. As one of the hot biofuels of fuel additives or alternative fuels, this paper selects the short chain methanol and the long chain 2- methyl -1- butanol as the research object, and analyzes the basic laws of the pyrolysis and combustion of alcohols. On the one hand, the methanol combustion model is optimized as the basic model for the study of alcohols combustion; the other side is the other side. On the basis of 2- methyl -1- butanol as the representative, the decomposition law of fuel in the combustion process of large molecular alcohol fuel is explored. The main contents of this study include two aspects of experiment and model study. The measurement of flame propagation velocity and the diagnosis of laminar premixed flame are carried out for methanol, and the macro combustion parameters and the number of micro reaction kinetics are taken into consideration. The laminar flame propagation velocity of methanol is measured by the experimental platform of the combustion bomb, the unburned premixed gas temperature is 423 K, the experimental combustion pressure condition is 1-10 atm. methanol in the laminar premixed flame experiment with the latest developed laminar premixed flame experimental platform, and the ultrasonic molecular beam sampling junction is used. The contract step radiation vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS) was developed to measure the concentration information of the stable products and active intermediates during the process of methanol combustion. The experimental pressure was 30Torr. The active 1.0. was carried out to study the pyrolysis of the active pentyl alcohol, and the concentration information of the primary products during the decomposition process was measured. The 2- methyl -1- butanol variable pressure flow tube pyrolysis experiment also uses ultrasonic molecular beam sampling combined with synchrotron vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS), experimental pressure conditions 30 and 760 Torr, and the temperature range is 750-1400 K.. Based on the previous experiments, theoretical calculation and model research data collection, this paper is constructed. The kinetic model of the combustion reaction of methanol was modeled and the CHEMKIN-PRO software was used to verify the literature and the experimental data. A good model of methanol was developed and optimized in a wide range of experimental conditions. At the same time, the pyrolysis model of 2- methyl -1- butanol was developed, and the pyrolysis of butanol isomers before this group was studied. The effects of carbon chain growth and branched chain structure on the pyrolysis of alcohols are discussed in detail. The specific results are as follows: first, the flame propagation velocity of the equivalent ratio of 0.7-2.1 is measured under 1-10 ATM of methanol by the combustion bomb experiment. By analyzing the reaction mechanism under the condition of high pressure and extremely rich combustion, the HO2 radical is high pressure and rich. The main free radicals in the flame propagation process are very sensitive to the prediction of the velocity of the flame propagation of the methanol under this condition. This work updates the reaction rate constant involving the H02 transformation in the hydrogen mechanism, and the formation and consumption of H02 in the mechanism of formaldehyde and methanol. These updates will bring the flame to the flame. The prediction of free radical pool in the propagation system has great influence, and it greatly improves the prediction of flame propagation velocity under high pressure and burning condition. Secondly, the SVUV-PIMS method has been used to identify the hydroxyl radical (CH2OH) and methoxy radical (CH30) which can not be distinguished by predecessors, and the quantitative measurement of hydroxymethyl free radical CH2OH is made. Based on the mole fraction information of CH2OH and the model study of other C1 products measured by the experiment, it is found that the predecessors overestimated the path of the formation of formaldehyde from the hydroxymethyl radical, that is, the reaction rate of CH2OH+O2=CH2O+HO2 was overestimated at high temperature. In addition, the results of this work proved that the former C2 species in the methanol model were found. Self methyl compound has very low efficiency. Therefore, this work explores the path of hydroxyl methyl free radical CH2OH composite generation of C2 species. The addition of these reaction paths greatly improves the prediction of C2 species. Finally, the SVUV-PIMS method is used to fully detect the pyrolysis of 2- methyl -1- butanol, and a 2- A is developed and verified. By comparing the pyrolysis of butanol isomer, we found that the pyrolysis mechanism of 2- methyl -1- butanol is similar to that of isobutanol, but it is very different from that of n-butanol. The contribution of the two kinds of branched alcohols in the pyrolysis of the two kinds of branched chain alcohols is much smaller than that of the H.
【學(xué)位授予單位】：中國(guó)科學(xué)技術(shù)大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2016
【分類(lèi)號(hào)】：TK16

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