汽油车冷起动挥发性有机物排放及生成机理的研究
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摘要
挥发性有机物(Volatile Organic Compounds, VOCs)是汽油车主要有害排放物之一,对人体健康和大气环境危害很大,而冷起动阶段汽油车VOCs排放恶劣。本文在国内外学者研究基础上,开发了一种汽车尾气采集系统,采集并检测了汽车尾气中VOCs,包括多环芳香烃(Polycyclic Aromatic Hydrocarbons,PAHs)、羰基化合物(Carbonyl Compounds)、细粒子(nano-particulate)等,重点研究了其在冷起动阶段各工况的排放特性;同时,利用KIVA-3V软件,对冷起动工况下碳氢化合物(HC)生成机理及排放规律进行了模拟研究。论文主要研究工作和结果如下:
1.基于常规的汽车尾气检测平台,开发了汽车尾气采集系统,该系统在按国III方法检测尾气常规排放的同时,可瞬时完成所需工况点的尾气采集,且能够连续采集多个工况点,便于对VOCs排放结果的分析、对比。根据汽油机尾气排放特点,针对不同组分的化学特性,设计了合理的尾气采集方案。
2.建立了汽油机VOCs主要有害排放物的前处理和检测方法,其中被检测PAHs的回收率大于90 %,相对标准偏差均低于15 %;醛酮类物质的平均回收率在96.07～99.99 %,各衍生物的相对标准偏差为0.193～0.409 %,具有较高的测试准确度,满足对于极低含量物质的检测。
3.汽油车起动工况下的VOCs排放量非常大,可达到10000ppm;按美国国家环保局(EPA)TO14、TO15标准,汽油车排放VOCs各组分中,芳香烃分担率很高,达50 %左右,其中以甲苯、二甲苯、三甲苯等所占比例较大;尾气中含有多环芳香烃,气态且环数较少的PAHs排放较高,如萘、苊、菲、芴等二环或三环组分,占PAHs的98 %左右;尾气中含大量细粒子,冷起动工况下直径小于1μm的粒子数量浓度可达到4.35x107个/cm3。
4.利用KIVA-3V软件,构建了一个新的异辛烷氧化反应的骨架机理和新的液滴碰撞模型(MIC),并将其添加到KIVA-3V软件的动力学反应模块中,模拟了不同缸内温度下HC的生成情况,研究了点火提前角、进气温度、点火能量等因素对冷起动HC生成和排放的影响。模拟计算结果显示,适当减小冷起动时的点火提前角,增加后燃,能迅速的提高缸内温度,可减少冷起动HC排放;提高进气温度和加大点火能量也是降低冷起动下HC排放的可用措施。
Volatile organic compounds (VOCs) as one kind of the main hazardous exhaust pollutants from gasoline passenger cars have a great hazard to the atmospheric environment and human health, and most of them emitted in cold-start phase. In this thesis, based on the former investigations, a novel sampling system was developed to quickly collect VOCs in the exhaust emissions, including polycyclic aromatic hydrocarbons (PAHs), carbonyl compounds(CBCs), nano-particulate and so on. With this system developed, the specific emphasis was lay upon the emission characteristics of VOCs during each stage of cold-start phase. Meanwhile, the formation mechanism of hydrocarbons (HC) in cold-start condition was simulated using KIVA-3V software. The main work and conclusions to the study are summarized as follows:
1. Based on the conventional automobile exhaust testing bed, a novel exhaust emissions sampling system was developed. The system can not only fulfill the collection of regulated exhaust emissions according to Stage III Standard, but also actualize to sample the VOCs at each applied operation mode expeditiously and consecutively. The collecting pattern of VOCs facilitates the contrast and analysis of the samples. In addition, the collecting programs were designed in accordance with the chemical characteristics of components in the gasoline engine exhaust emissions.
2. New pretreatment and analytical methods were established to detect the hazardous components in the VOCs from a gasoline passenger car. By means of the methods, the recovery rate of PAHs exceeds 90 % with the relative standard deviation (RSD) less than 15 %, the average recovery of CBCs ranges from 96.07 % to 99.99 % with the RSD in the range of 0.193 % - 0.409 %. The results prove that the accuracy of analytical methods is high enough to detect the trace substances in the engine exhaust emissions.
3. The VOCs have a so high content in the exhaust emissions from the gasoline passenger car during the cold-start period as to reach 10000ppm. According to the EPA TO-14/TO-15 methods, aromatic hydrocarbons are the major sort in the VOCs, and account for approximately 50 %. Toluene, xylene and trimethylbenzene are the most predominant components in aromatic hydrocarbons. PAHs are also found in the exhaust emissions, and the 2-ring or 3-ring aromatics such as naphthalene, acenaphthene, phenanthrene and fluorene are the PAHs quantified in higher concentration and share about 98 % of PAHs. A large number of nano-particulates were detected in the engine exhaust emissions by electrical low-pressure impactor (ELPI), and the number concentration of particulates with the aerodynamics diameter less than 1μm can reach 4.35x107 (1/cm3) in cold-start phase.
4. In order to study the generation and evolution of hydrocarbons in the cold-start condition, a new framework mechanism of isooctane oxidation reaction and a new mesh independent collision (MIC) spray drop collision model were constructed and added to the overall dynamic reaction of KIVA-3V. The effect of several parameters, such as ignition advance angle, inlet temperature, ignition energy, on HC generation in cold-start phase of the gasoline engine were studied. The simulation results show that the reasonable decrease in ignition advance angle during cold-start period can increase after-burning, and then raise the cylinder’s temperature quickly, reducing cold-start HC emissions. Also, enhancing the intake air temperature and ignition energy are the feasible approach to reducing the cold-start HC emissions.
1.基于常规的汽车尾气检测平台,开发了汽车尾气采集系统,该系统在按国III方法检测尾气常规排放的同时,可瞬时完成所需工况点的尾气采集,且能够连续采集多个工况点,便于对VOCs排放结果的分析、对比。根据汽油机尾气排放特点,针对不同组分的化学特性,设计了合理的尾气采集方案。
2.建立了汽油机VOCs主要有害排放物的前处理和检测方法,其中被检测PAHs的回收率大于90 %,相对标准偏差均低于15 %;醛酮类物质的平均回收率在96.07～99.99 %,各衍生物的相对标准偏差为0.193～0.409 %,具有较高的测试准确度,满足对于极低含量物质的检测。
3.汽油车起动工况下的VOCs排放量非常大,可达到10000ppm;按美国国家环保局(EPA)TO14、TO15标准,汽油车排放VOCs各组分中,芳香烃分担率很高,达50 %左右,其中以甲苯、二甲苯、三甲苯等所占比例较大;尾气中含有多环芳香烃,气态且环数较少的PAHs排放较高,如萘、苊、菲、芴等二环或三环组分,占PAHs的98 %左右;尾气中含大量细粒子,冷起动工况下直径小于1μm的粒子数量浓度可达到4.35x107个/cm3。
4.利用KIVA-3V软件,构建了一个新的异辛烷氧化反应的骨架机理和新的液滴碰撞模型(MIC),并将其添加到KIVA-3V软件的动力学反应模块中,模拟了不同缸内温度下HC的生成情况,研究了点火提前角、进气温度、点火能量等因素对冷起动HC生成和排放的影响。模拟计算结果显示,适当减小冷起动时的点火提前角,增加后燃,能迅速的提高缸内温度,可减少冷起动HC排放;提高进气温度和加大点火能量也是降低冷起动下HC排放的可用措施。
Volatile organic compounds (VOCs) as one kind of the main hazardous exhaust pollutants from gasoline passenger cars have a great hazard to the atmospheric environment and human health, and most of them emitted in cold-start phase. In this thesis, based on the former investigations, a novel sampling system was developed to quickly collect VOCs in the exhaust emissions, including polycyclic aromatic hydrocarbons (PAHs), carbonyl compounds(CBCs), nano-particulate and so on. With this system developed, the specific emphasis was lay upon the emission characteristics of VOCs during each stage of cold-start phase. Meanwhile, the formation mechanism of hydrocarbons (HC) in cold-start condition was simulated using KIVA-3V software. The main work and conclusions to the study are summarized as follows:
1. Based on the conventional automobile exhaust testing bed, a novel exhaust emissions sampling system was developed. The system can not only fulfill the collection of regulated exhaust emissions according to Stage III Standard, but also actualize to sample the VOCs at each applied operation mode expeditiously and consecutively. The collecting pattern of VOCs facilitates the contrast and analysis of the samples. In addition, the collecting programs were designed in accordance with the chemical characteristics of components in the gasoline engine exhaust emissions.
2. New pretreatment and analytical methods were established to detect the hazardous components in the VOCs from a gasoline passenger car. By means of the methods, the recovery rate of PAHs exceeds 90 % with the relative standard deviation (RSD) less than 15 %, the average recovery of CBCs ranges from 96.07 % to 99.99 % with the RSD in the range of 0.193 % - 0.409 %. The results prove that the accuracy of analytical methods is high enough to detect the trace substances in the engine exhaust emissions.
3. The VOCs have a so high content in the exhaust emissions from the gasoline passenger car during the cold-start period as to reach 10000ppm. According to the EPA TO-14/TO-15 methods, aromatic hydrocarbons are the major sort in the VOCs, and account for approximately 50 %. Toluene, xylene and trimethylbenzene are the most predominant components in aromatic hydrocarbons. PAHs are also found in the exhaust emissions, and the 2-ring or 3-ring aromatics such as naphthalene, acenaphthene, phenanthrene and fluorene are the PAHs quantified in higher concentration and share about 98 % of PAHs. A large number of nano-particulates were detected in the engine exhaust emissions by electrical low-pressure impactor (ELPI), and the number concentration of particulates with the aerodynamics diameter less than 1μm can reach 4.35x107 (1/cm3) in cold-start phase.
4. In order to study the generation and evolution of hydrocarbons in the cold-start condition, a new framework mechanism of isooctane oxidation reaction and a new mesh independent collision (MIC) spray drop collision model were constructed and added to the overall dynamic reaction of KIVA-3V. The effect of several parameters, such as ignition advance angle, inlet temperature, ignition energy, on HC generation in cold-start phase of the gasoline engine were studied. The simulation results show that the reasonable decrease in ignition advance angle during cold-start period can increase after-burning, and then raise the cylinder’s temperature quickly, reducing cold-start HC emissions. Also, enhancing the intake air temperature and ignition energy are the feasible approach to reducing the cold-start HC emissions.
引文
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