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

【摘要】：能源是國民經(jīng)濟的動力和命脈�；剂系娜紵峁┝巳�85%和我國近90%的一次能源需求。現(xiàn)如今化石燃料的急劇消耗不僅帶來了前所未有的能源危機,還釀成了環(huán)境污染的惡果,時刻威脅著環(huán)境安全和人類健康。生物醇類,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對化石燃料的過分依賴,另一方面醇類燃料中的C02排放和吸收構(gòu)成自然界碳循環(huán),可實現(xiàn)C02近零排放。目前,國際上對生物醇類的研究涵蓋C1-C8的醇類。其中甲醇是最簡單的醇類,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的模型燃料,因此,對甲醇燃料燃燒反應(yīng)動力學(xué)進行深入研究具有重要意義。作為長鏈醇類的代表之一,2-甲基-1-丁醇(活性戊醇)是一種含有5個碳原子的醇類,相比分子量較小的甲醇,它表現(xiàn)出諸多明顯的優(yōu)勢,比如：能量密度大,具有較低蒸汽壓,疏水性強,可與碳氫化合物很好互溶等,因此2-甲基-1-丁醇非常適合作為運輸燃料,是不久的將來能作為實際輸運燃料中添加劑或替代燃料的熱門生物燃料之一。因此,本論文選擇短鏈的甲醇和長鏈的2-甲基-1-丁醇作為研究對象,深入分析醇類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,探索大分子醇類燃料燃燒過程中燃料的分解規(guī)律。本文的研究內(nèi)容主要包括實驗和模型研究兩大方面,對甲醇開展了火焰?zhèn)鞑ニ俣鹊臏y量和層流預(yù)混火焰的診斷實驗,兼顧宏觀燃燒參數(shù)和微觀反應(yīng)動力學(xué)數(shù)據(jù)的采集。甲醇的層流火焰?zhèn)鞑ニ俣葴y量利用了本組的燃燒彈實驗平臺,未燃預(yù)混燃氣溫度為423 K,實驗測量的燃燒壓力條件為1-10 atm。甲醇的層流預(yù)混火焰實驗借助本組最新研制出的層流預(yù)混火焰實驗平臺,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,測量了甲醇燃燒過程中穩(wěn)定產(chǎn)物以及活潑中間體的濃度信息,實驗壓力30Torr,當(dāng)量1.0。本工作對活性戊醇開展了變壓力的流動管熱解研究,重點測量其分解過程中初級產(chǎn)物的濃度信息。2-甲基-1-丁醇的變壓力流動管熱解實驗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),實驗壓力條件30和760 Torr,溫度范圍在750-1400 K。此外,基于對前人實驗、理論計算和模型研究數(shù)據(jù)的全面收集,本文構(gòu)建了甲醇的燃燒反應(yīng)動力學(xué)模型,并利用CHEMKIN-PRO軟件對文獻和本文實驗數(shù)據(jù)進行了驗證,發(fā)展并優(yōu)化了一個能夠在寬廣實驗工況下預(yù)測良好的甲醇模型。同時,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)體的熱解進行詳細對比,探討了碳鏈增長和支鏈結(jié)構(gòu)對醇類燃料熱解的影響。具體研究成果如下：首先,通過燃燒彈實驗,測量了甲醇1-10 atm下,當(dāng)量比為0.7-2.1的火焰?zhèn)鞑ニ俣取Ｍㄟ^分析高壓和極富燃條件下的反應(yīng)機制發(fā)現(xiàn),HO2自由基是高壓和富燃條件下火焰?zhèn)鞑ミ^程中的主要自由基,與它相關(guān)的反應(yīng)在該條件下對甲醇火焰?zhèn)鞑ニ俣鹊念A(yù)測非常敏感。本工作更新了氫氣機理中涉及H02轉(zhuǎn)化的反應(yīng)速率常數(shù),以及甲醛和甲醇子機理中H02的生成和消耗反應(yīng)速率,這些更新會對火焰?zhèn)鞑ンw系自由基池的預(yù)測帶來較大影響,同時大大改善了前人模型對高壓和富燃條件下火焰?zhèn)鞑ニ俣鹊念A(yù)測。其次,利用SVUV-PIMS方法鑒別了前人無法區(qū)分的羥甲基自由基(CH2OH)和甲氧基自由基(CH30),并對羥甲基自由基CH2OH進行定量測量�；贑H2OH的摩爾分數(shù)信息,以及實驗測得的其它C1產(chǎn)物進行模型研究,發(fā)現(xiàn)前人過高估計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,通過本工作的實驗結(jié)果驗證,發(fā)現(xiàn)前人的甲醇模型中C2物種來自甲基復(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C2物種的預(yù)測情況。最后,利用SVUV-PIMS方法,對2-甲基-1-丁醇的熱解中間體進行全面探測,發(fā)展并驗證了一個2-甲基-1-丁醇的熱解模型。通過對比丁醇異構(gòu)體熱解規(guī)律,我們發(fā)現(xiàn)2-甲基-1-丁醇的熱解機制與異丁醇的熱解機制相近,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)的貢獻比H提取反應(yīng)的貢獻要小很多的特點。
[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】：中國科學(xué)技術(shù)大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2016
【分類號】：TK16

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