乙醇/生物柴油燃烧过程试验研究与理论分析
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摘要
乙醇和生物柴油作为柴油机的替代燃料,得到了越来越广泛的关注和应用。乙醇、生物柴油与柴油的组成、分子结构不同,理化特性存在差异。这些燃料的理化特性也会影响燃烧过程和燃烧产物。论文围绕含氧燃料和石化燃料的燃烧过程及其生成的颗粒物开展了研究工作,针对乙醇、生物柴油与柴油的组分和分子结构特点,采用分子杂化轨道理论,运用相似相溶和溶剂化观点,对生物柴油可以提高乙醇与柴油互溶的机理进行了解释；从极性作用力的角度,探讨了乙醇、生物柴油对柴油机橡胶燃油管的腐蚀机理。在含氧燃料燃烧过程的的研究中,采用同步辐射燃烧试验装置、预混燃烧器、柴油机台架装置,研究含氧燃料不同燃烧方式的燃烧速率、温度、产物,示功图等的变化规律；针对含氧燃料燃烧方式的不同,建立了仿真模型,研究含氧燃料燃烧过程中自由基的变化特征、中间产物的生成特性及含氧燃料中氧元素的迁移路径；开展了含氧燃料分子结构特征与燃烧产物形成机理的研究；采用扫描电镜和同步辐射小角X散射装置表征了乙醇和生物柴油燃烧颗粒物的几何尺寸和微区结构。主要结论如下：
对不同温度、不同比例的乙醇在柴油中的溶解进行了试验研究,采用生物柴油做为助溶剂,探讨了生物柴油增大乙醇在柴油中的溶解机理,结果表明：生物柴油分子一方面与柴油分子中的烃分子通过范德华力作用结合,另一方面通过极性分子作用与乙醇分子结合,结果表明生物柴油具有两向亲和作用,可以增大乙醇在柴油中的溶解能力。
对柴油机燃油供给系中主要材料了腈橡胶的腐蚀溶胀进行了研究,采用浸泡和电镜扫描的试验方法,考察了橡胶管在乙醇、生物柴油中浸泡672小时前后的质量、体积、硬度等参数的变化,拍摄了橡胶管内表面照片,并与柴油进行了对比,分析分子极性作用力在燃汕和橡胶中的作用过程。结果表明：含氧燃料对丁腈橡胶有腐蚀溶胀作用。乙醇的极性最强,对丁腈橡胶的腐蚀最为强烈,提出了燃料分子的极性力是造成含氧燃料腐蚀柴油机燃油橡胶管的观点。
应用同步辐射燃烧试验、常温常压预混和柴油机台架的试验方法,研究了不同压力、不同当量比、不同掺混比乙醇、生物柴油的燃烧过程,并与燃用柴油的燃烧过程进行了比较；分析了添加乙醇、生物柴汕对柴油机燃油过程及产物的影响,通过试验研究得到：燃料和空气混合的方式不同,当量比不同,燃烧速率就有区别,乙醇可以增大乙醇/柴油燃烧速率；乙醇的预混燃烧外焰、中焰、内焰温度分别是扩散燃烧的1.8、1.5、1.96倍,乙醇、生物柴汕在柴油机上燃烧降低颗粒物的效果明显,对NOx的影响较小。
运用层流预混火焰反应器模型,提出了从化学反应动力学角度,采用反应生成率和敏感性分析方法,考察了柴油、乙醇和生物柴油的主要反应路径、自由基和中间体的生成特性,重点研究了含氧燃料中O元素的迁移途径,探讨了物柴汕燃烧过程中甲酯基的裂解路径。结果农明：燃料燃烧产：物中烯烃的摩尔分数大于同类的烷烃和炔烃,提出了乙醇燃烧过程中,乙醇分子经过脱氢、裂解,最终生成H2O、CO的观点；也提出了大分子生物柴汕甲酯基在自由基的进攻下,不同位置失去氢原子转化为不同的甲醛基,进一步失去C2H4生成奇数碳和偶数碳的裂解产物,奇数碳甲酯基燃烧产物摩尔分数大于偶数碳甲酯基的观点。
考察了不同含氧量混合燃料的HCCI燃烧,探讨了温度、自由基摩尔分数随含氧量的变化规律。研究农明：曲轴转角上止点附近,自由基迅速生成并快速消耗,反应放出大量的热,温度度迅速升高。随掺混含氧燃料比例的增大,缸内温度下降,自由基摩尔分数峰值依次后移。
研究了乙醇和其同分异构体二甲醚的预混燃烧过程,确定了燃烧过程中乙醇和二甲醚的反应速率,烯烃、炔烃的关键生成反应,结合了乙醇和二甲醚的分子结构特点,确定了乙醇可以直接裂解生成C2H4,二甲醚先经过脱氢,碳氧键断裂,最终聚合为C2H4的衍生过程,对乙醇和二甲醚中影响C2H4的敏感性进行了详细的解释。
通过分析生物柴油裂解的路径、芳香烃苯的形成过程,结合生物柴油分子的结构特点,提出了从化学动力学方面,考察生物柴油芳香烃物质形成过程的影响因素,探讨了生物柴油的含氧量、饱和度、碳链长度对苯的影响规律。
采集了常温常压下的不同比例的乙醇/生物柴油燃烧颗粒物的样本,采用扫描电子显微镜、同步辐射小角X散射测量的方法,从电子密度属性方面探讨含氧燃料燃烧颗粒物的微区结构和几何尺寸,总结了颗粒物的变化规律。研究表明,柴油中添加含氧燃料,随含氧燃料的增加,燃烧颗粒物粒径变小,回转半径和平均半径减小,平均界面厚度减小。颗粒物的Porod曲线都呈负偏离,颗粒和分散介质间的界面模糊,存在界面层。
Ethanol and biodiesel, as alternative fuels of diesel engine, have been widely concerned and used. The composition and molecular structure of ethanol, biodiesel are different from diesel, leading the difference of physical and chemical properties which influence the combustion process and combustion products. In this paper, the combustion process and particulate matter(PM) of oxygenated fuel and fossil fuel have been studied. According to the characteristics of component and molecularstructure of ethanol, biodiesel, diesel, based on the theory of molecular hybrid orbital, similarity and intermiscibility, and solvation, the mechanism that biodiesel can improve the mutual solubility of ethanol and diesel was explained. Besides, the corrosion mechanism of rubber fuel tube of diesel engine in ethanol and biodiesel was explored from the perspective of polar force. Synchrotron radiation, premix burner and diesel engine in bench test were adopted in the study of combustion process. Changing laws of burning rate, temperature, combustion products and indicator diagram under different combustion mode were studied. According to different combustion modes, the simulation model was established to research free radical variation characteristic, producing characteristic of intermediate products and migration path of oxygen in combustion progress. The molecular structure of oxygenated fuels and formation mechanism combustion products were studied. SEM (scanning electron microscope) and synchrotron radiation small angle X-ray scattering were used to characterize the geometry size and PM micro-region structure of ethanol and biodiesel. The main conclusions are following:
Solubility in diesel of ethanol with different proportion, at different temperature was tested. Biodiesel was used as cosolvent of ethanol and diesel, and the cosolvent mechanism was studied. Results showed that biodiesel molecule combined diesel molecule by Vad der Waals force on one hand, and combined ethanol molecule polar force on the other hand. Therefore, biodiesel molecule played a role as bidirectional affinity interaction to improve the solubility of ethanol in diesel.
The corrosion and swelling performance of nitrile rubber which is the main material of diesel engine fuel injection system was studied by soak and SEM. Parameters like mass, volume and hardness before and after soaking in ethanol, biodiesel for672hours were studied. Inner surface of the rubber tube soaked in ethanol, biodiesel and diesel was photographed, and the action process of polar force in rubber was analyzed. Results showed that oxygenated fuels corroded and swelled nitrile rubber. Ethanol which had the strongest polar force corroded nitrile rubber most. Molecule polar force of oxygenated fuel was the reason that corroded rubber tube.
The combustion process of ethanol, biodiesel, diesel under different pressure, different equivalence ratio and different blending ratio was studied, using the method of synchrotron radiation, normal pressure and temperature premixed and diesel engine bench test. The influence of ethanol, biodiesel in blends on combustion process and products was analyzed. Results showed that oil and gas mixing mode, equivalent ratio influenced the burned rate. Ethanol can improve the burning rate of ethanol/diesel. The ethanol premixed combustion temperature of outer flame, intermediate flame, and inner flame were respectively1.8,1.5and1.96times higher than diffusion combustion. Ethanol, biodiesel used in diesel engine can significantly reduce PM, but did influence NOX too much.
Using laminar premixed flame reactor model, from the perspective of chemical reaction kinetics, the main reaction paths, free radicals and intermediate products producing characteristic of diesel, ethanol and biodiesel were studied by means of reaction rate and sensitivity analysis.The paper focused on the pathways of oxygen in oxygenated fuels to analyze the cracking paths of carbomethoxy in the combustion process of biodiesel. Results showed that the mole fraction of olefins was larger than kindred alkane and alkyne of combustion products. The point that ethanol generated into H2O, CO after dehydrogenation, cracking was proposed. The other point was also proposed that with the attack of free radicals, the biodiesel macromolecule would lose hydrogenatom at different positions and turn into different kinds of carbomethoxy, then lose C2H4further, turning into cracking products with odd and even carbon. And mole fraction of carbomethoxy with odd carbon was larger than carbomethoxy with even carbon.
HCCI combustion of blends with different oxygen content was investigated. The variation law of temperature and free radicals were discussed. Results showed that free radicals were generated and consumed quickly near TDC, lots of heat was released and the temperature increased rapidly. With the increase of oxygenated fuel proportion, the in-cylinder temperature decreased, and the phase of peak mole fraction of radicals postponed.
DME is the isomer of ethanol. The premixed combustion of ethanol and DME were studied to determine the reaction rate in the combustion process, and the key formation reaction of olefins and alkyne. According to the molecule structure characteristics of ethanol and DME, it was found that ethanol can be directly cracked into C2H4, while DME would firstly be dehydrogenized, then C-O bonds broken, and eventually polymerized into C2H4. A detail explanation about the influence caused by ethanol and DME on the, sensitivity of C2H4formation was given.
After analyzing biodiesel cracking paths and formation process of aromatic hydrocarbon benzene, combining the biodiesel molecule structure, the influencing factors of formation process of biodiesel was proposed from the perspective of chemical kinetics. The influence law of oxygen content, saturation and carbon chain length of biodiesel on benzene formation were discussed.
Examples of combustion particulate matter of ethanol/biodiesel with different proportional under normal pressure and temperature were collected. The geometry size and micro-region structure of combustion particulate matter of oxygenated fuels were studied from the perspective of electron density properties, by the method of SEM and synchrotron radiation small angle X-ray scattering, and got the variation law of particulate matter. Results showed that with the increase of oxygenated fuel proportion, the size of combustion particulate matter decreased, the gyration radius and the mean radius reduced and the average thickness of the interface lowered. The Porod curve of particulate matter was negative deflected, and the interface between particulate matter and dispersion medium was fuzzy, indicating that interface layers were existent.
对不同温度、不同比例的乙醇在柴油中的溶解进行了试验研究,采用生物柴油做为助溶剂,探讨了生物柴油增大乙醇在柴油中的溶解机理,结果表明：生物柴油分子一方面与柴油分子中的烃分子通过范德华力作用结合,另一方面通过极性分子作用与乙醇分子结合,结果表明生物柴油具有两向亲和作用,可以增大乙醇在柴油中的溶解能力。
对柴油机燃油供给系中主要材料了腈橡胶的腐蚀溶胀进行了研究,采用浸泡和电镜扫描的试验方法,考察了橡胶管在乙醇、生物柴油中浸泡672小时前后的质量、体积、硬度等参数的变化,拍摄了橡胶管内表面照片,并与柴油进行了对比,分析分子极性作用力在燃汕和橡胶中的作用过程。结果表明：含氧燃料对丁腈橡胶有腐蚀溶胀作用。乙醇的极性最强,对丁腈橡胶的腐蚀最为强烈,提出了燃料分子的极性力是造成含氧燃料腐蚀柴油机燃油橡胶管的观点。
应用同步辐射燃烧试验、常温常压预混和柴油机台架的试验方法,研究了不同压力、不同当量比、不同掺混比乙醇、生物柴油的燃烧过程,并与燃用柴油的燃烧过程进行了比较；分析了添加乙醇、生物柴汕对柴油机燃油过程及产物的影响,通过试验研究得到：燃料和空气混合的方式不同,当量比不同,燃烧速率就有区别,乙醇可以增大乙醇/柴油燃烧速率；乙醇的预混燃烧外焰、中焰、内焰温度分别是扩散燃烧的1.8、1.5、1.96倍,乙醇、生物柴汕在柴油机上燃烧降低颗粒物的效果明显,对NOx的影响较小。
运用层流预混火焰反应器模型,提出了从化学反应动力学角度,采用反应生成率和敏感性分析方法,考察了柴油、乙醇和生物柴油的主要反应路径、自由基和中间体的生成特性,重点研究了含氧燃料中O元素的迁移途径,探讨了物柴汕燃烧过程中甲酯基的裂解路径。结果农明：燃料燃烧产：物中烯烃的摩尔分数大于同类的烷烃和炔烃,提出了乙醇燃烧过程中,乙醇分子经过脱氢、裂解,最终生成H2O、CO的观点；也提出了大分子生物柴汕甲酯基在自由基的进攻下,不同位置失去氢原子转化为不同的甲醛基,进一步失去C2H4生成奇数碳和偶数碳的裂解产物,奇数碳甲酯基燃烧产物摩尔分数大于偶数碳甲酯基的观点。
考察了不同含氧量混合燃料的HCCI燃烧,探讨了温度、自由基摩尔分数随含氧量的变化规律。研究农明：曲轴转角上止点附近,自由基迅速生成并快速消耗,反应放出大量的热,温度度迅速升高。随掺混含氧燃料比例的增大,缸内温度下降,自由基摩尔分数峰值依次后移。
研究了乙醇和其同分异构体二甲醚的预混燃烧过程,确定了燃烧过程中乙醇和二甲醚的反应速率,烯烃、炔烃的关键生成反应,结合了乙醇和二甲醚的分子结构特点,确定了乙醇可以直接裂解生成C2H4,二甲醚先经过脱氢,碳氧键断裂,最终聚合为C2H4的衍生过程,对乙醇和二甲醚中影响C2H4的敏感性进行了详细的解释。
通过分析生物柴油裂解的路径、芳香烃苯的形成过程,结合生物柴油分子的结构特点,提出了从化学动力学方面,考察生物柴油芳香烃物质形成过程的影响因素,探讨了生物柴油的含氧量、饱和度、碳链长度对苯的影响规律。
采集了常温常压下的不同比例的乙醇/生物柴油燃烧颗粒物的样本,采用扫描电子显微镜、同步辐射小角X散射测量的方法,从电子密度属性方面探讨含氧燃料燃烧颗粒物的微区结构和几何尺寸,总结了颗粒物的变化规律。研究表明,柴油中添加含氧燃料,随含氧燃料的增加,燃烧颗粒物粒径变小,回转半径和平均半径减小,平均界面厚度减小。颗粒物的Porod曲线都呈负偏离,颗粒和分散介质间的界面模糊,存在界面层。
Ethanol and biodiesel, as alternative fuels of diesel engine, have been widely concerned and used. The composition and molecular structure of ethanol, biodiesel are different from diesel, leading the difference of physical and chemical properties which influence the combustion process and combustion products. In this paper, the combustion process and particulate matter(PM) of oxygenated fuel and fossil fuel have been studied. According to the characteristics of component and molecularstructure of ethanol, biodiesel, diesel, based on the theory of molecular hybrid orbital, similarity and intermiscibility, and solvation, the mechanism that biodiesel can improve the mutual solubility of ethanol and diesel was explained. Besides, the corrosion mechanism of rubber fuel tube of diesel engine in ethanol and biodiesel was explored from the perspective of polar force. Synchrotron radiation, premix burner and diesel engine in bench test were adopted in the study of combustion process. Changing laws of burning rate, temperature, combustion products and indicator diagram under different combustion mode were studied. According to different combustion modes, the simulation model was established to research free radical variation characteristic, producing characteristic of intermediate products and migration path of oxygen in combustion progress. The molecular structure of oxygenated fuels and formation mechanism combustion products were studied. SEM (scanning electron microscope) and synchrotron radiation small angle X-ray scattering were used to characterize the geometry size and PM micro-region structure of ethanol and biodiesel. The main conclusions are following:
Solubility in diesel of ethanol with different proportion, at different temperature was tested. Biodiesel was used as cosolvent of ethanol and diesel, and the cosolvent mechanism was studied. Results showed that biodiesel molecule combined diesel molecule by Vad der Waals force on one hand, and combined ethanol molecule polar force on the other hand. Therefore, biodiesel molecule played a role as bidirectional affinity interaction to improve the solubility of ethanol in diesel.
The corrosion and swelling performance of nitrile rubber which is the main material of diesel engine fuel injection system was studied by soak and SEM. Parameters like mass, volume and hardness before and after soaking in ethanol, biodiesel for672hours were studied. Inner surface of the rubber tube soaked in ethanol, biodiesel and diesel was photographed, and the action process of polar force in rubber was analyzed. Results showed that oxygenated fuels corroded and swelled nitrile rubber. Ethanol which had the strongest polar force corroded nitrile rubber most. Molecule polar force of oxygenated fuel was the reason that corroded rubber tube.
The combustion process of ethanol, biodiesel, diesel under different pressure, different equivalence ratio and different blending ratio was studied, using the method of synchrotron radiation, normal pressure and temperature premixed and diesel engine bench test. The influence of ethanol, biodiesel in blends on combustion process and products was analyzed. Results showed that oil and gas mixing mode, equivalent ratio influenced the burned rate. Ethanol can improve the burning rate of ethanol/diesel. The ethanol premixed combustion temperature of outer flame, intermediate flame, and inner flame were respectively1.8,1.5and1.96times higher than diffusion combustion. Ethanol, biodiesel used in diesel engine can significantly reduce PM, but did influence NOX too much.
Using laminar premixed flame reactor model, from the perspective of chemical reaction kinetics, the main reaction paths, free radicals and intermediate products producing characteristic of diesel, ethanol and biodiesel were studied by means of reaction rate and sensitivity analysis.The paper focused on the pathways of oxygen in oxygenated fuels to analyze the cracking paths of carbomethoxy in the combustion process of biodiesel. Results showed that the mole fraction of olefins was larger than kindred alkane and alkyne of combustion products. The point that ethanol generated into H2O, CO after dehydrogenation, cracking was proposed. The other point was also proposed that with the attack of free radicals, the biodiesel macromolecule would lose hydrogenatom at different positions and turn into different kinds of carbomethoxy, then lose C2H4further, turning into cracking products with odd and even carbon. And mole fraction of carbomethoxy with odd carbon was larger than carbomethoxy with even carbon.
HCCI combustion of blends with different oxygen content was investigated. The variation law of temperature and free radicals were discussed. Results showed that free radicals were generated and consumed quickly near TDC, lots of heat was released and the temperature increased rapidly. With the increase of oxygenated fuel proportion, the in-cylinder temperature decreased, and the phase of peak mole fraction of radicals postponed.
DME is the isomer of ethanol. The premixed combustion of ethanol and DME were studied to determine the reaction rate in the combustion process, and the key formation reaction of olefins and alkyne. According to the molecule structure characteristics of ethanol and DME, it was found that ethanol can be directly cracked into C2H4, while DME would firstly be dehydrogenized, then C-O bonds broken, and eventually polymerized into C2H4. A detail explanation about the influence caused by ethanol and DME on the, sensitivity of C2H4formation was given.
After analyzing biodiesel cracking paths and formation process of aromatic hydrocarbon benzene, combining the biodiesel molecule structure, the influencing factors of formation process of biodiesel was proposed from the perspective of chemical kinetics. The influence law of oxygen content, saturation and carbon chain length of biodiesel on benzene formation were discussed.
Examples of combustion particulate matter of ethanol/biodiesel with different proportional under normal pressure and temperature were collected. The geometry size and micro-region structure of combustion particulate matter of oxygenated fuels were studied from the perspective of electron density properties, by the method of SEM and synchrotron radiation small angle X-ray scattering, and got the variation law of particulate matter. Results showed that with the increase of oxygenated fuel proportion, the size of combustion particulate matter decreased, the gyration radius and the mean radius reduced and the average thickness of the interface lowered. The Porod curve of particulate matter was negative deflected, and the interface between particulate matter and dispersion medium was fuzzy, indicating that interface layers were existent.
引文
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