压燃式发动机颗粒物排放理化特性及其对大气环境的影响
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摘要
高浓度的大气悬浮颗粒物对大气能见度、人体健康及气候变化均有着严重的影响，随着我国机动车保有量的不断增长，机动车颗粒物排放已成为城市大气悬浮颗粒物的重要来源。对机动车排气颗粒物理化特性的研究是正确认识颗粒物生成机理及其环境健康效应的基础，并可为判断大气悬浮颗粒物的污染来源，进而制定污染排放控制措施提供科学的依据。本文分别基于台架实验和道路实验两种方法对机动车颗粒物排放的理化特性做了系统深入的研究，并进一步提出了新的针对道路微环境下不同车型机动车颗粒物排放因子的计算方法，主要研究内容如下：
（1）针对超低硫柴油、低硫柴油和生物柴油三种不同燃料，在台架实验条件下，采用基于数量和质量两种不同方法研究了压燃式发动机排气颗粒物挥发性及其粒径分布特征。研究表明，相对低硫柴油，燃用生物柴油可以有效降低发动机排气颗粒中挥发性成分的比排放率，然而相对超低硫柴油，燃用生物柴油所产生颗粒物中挥发性物质成分的比排放率有所增加，其挥发性物质成分主要集中在小尺寸颗粒物中。
（2）研究了不同发动机工况、不同动力学粒径、不同燃油条件下发动机排气颗粒物形态、内部纳米结构及氧化活性。研究发现，发动机颗粒物的氧化活性主要取决于颗粒物基本粒子尺寸、挥发性物质比例及内部纳米结构特征等。由于燃用生物柴油所产生颗粒物较小的基本粒子尺寸、较高的挥发性物质比例以及相对短小、扭曲的内部碳层结构，其在热重实验中表现出相对超低硫柴油、低硫柴油颗粒物更强的氧化活性，与此同时，颗粒物的基本粒子尺寸、挥发性及内部碳层结构又与缸内燃烧条件、动力学粒径有着密切的关系。
（3）通过台架实验，研究了不同发动机负荷、不同动力学粒径以及燃油特性对颗粒物主要成分的影响，成分研究内容主要包括有机碳、元素碳及16种多环芳烃。试验结果表明，燃用生物柴油对颗粒物排放的抑制效果主要表现在燃烧生成的成分，如元素碳、大分子量的多环芳烃等，同时颗粒物的主要成分亦存在着明显的负荷变化及粒径分布特征。
（4）选取了上海地区一条典型的高速公路，开展了机动车排气颗粒对大气环境影响的研究，分别考察了白天和晚上道路微环境下大气悬浮颗粒物的理化特性，并与背景样品做了对比，主要测试内容包括不同粒径颗粒物的形貌、质量浓度及所包含的有机碳、元素碳、水溶性离子及多环芳烃的质量浓度。实验发现机动车对环境颗粒物的影响主要集中在<400nm的粒径范围内，在颗粒物主要成分中，机动车排放对元素碳、硝酸盐及多环芳烃浓度的影响最为明显。基于台架实验所获得的柴油发动机的排放源特征，采用正交矩阵因子法对路边颗粒物样品的主要成分进行源解析研究，得出不同车型机动车（柴油车、汽油车）排放对路边大气颗粒物的贡献比例，并据此改进了基于燃油消耗机动车颗粒物排放因子的计算方法，得出了不同车型机动车排放因子。计算结果表明，柴油车颗粒物排放是道路微环境下大气悬浮颗粒物的最主要贡献者，尤其对超细颗粒物的贡献达到60%以上。上海地区现行柴油车辆的颗粒物排放因子相对一些发达国家和地区仍处于一个比较高的水平。
Increased level of atmospheric aerosol can severely impact atmosphere visibility, publichealth and climate. With the rapid increase of vehicles in China, particulate emission has beenbecome one of the most important pollutant sources for atmospheric aerosol. Acomprehensive knowledge on physicochemical characteristics of vehicle particulate emissionis required to understand particle formation mechanism, hazards to the atmosphereenvironment, source assignment and ways to reduce particulate emission from motor vehicles.In this dissertation work, detailed physicochemical characteristics of particulate emissionwere investigated by dynamometry and roadside sampling. For the roadside experiment, anew method was proposed to calculate the vehicle emission factor with different engine types.This thesis is composed of the following parts:
(1) In the dynamometer experiment, ultra low sulfur diesel fuel (ULSD, sulfur contentless than10ppm), biodiesel (BD) and low sulfur diesel fuel (LSD, sulfur content lessthan400ppm) were used as the fuels. Detailed physicochemical characteristicsincluding size-dependent particle volatility, particle morphology, nanostructure,oxidation property and major composition were investigated. The size-dependentvolatility was investigated on the basis of number and mass measurements. It wasfound that, the use of biodiesel could reduce the brake specific emission of volatilesubstance effectively in comparison with LSD. While volatile substances in thebiodiesel particulate are notably greater than ULSD particulates and moreconcentrated in the particulates with small size.
(2) Particle morphology, nanostructure and oxidation property were also investigated overranges of engine operation conditions, aerodynamic sizes, and fuel types. Theoxidation experiments suggest that the oxidation property of diesel particulate dependon the primary particle size, volatile fraction, and nanostructure. Due to the smallerprimary particle size, larger volatile content and greater disordered inner nanostructure,biodiesel particulate exhibite stronger tendenty to oxidation than those from ULSDand LSD. Moreover, in-cylinder combustion parameter and fuel properties control theprimary particle size, volatile content and inner nanostructure of diesel particles.
(3) Analysis of particle composition included organic carbon, element carbon andpolycyclic aromatic hydrocarbons. In this thesis, the effect of engine load,aerodynamic size and fuel type on particle composition were investigated. The use ofbiodiesel appears to reduce particulate emissions from diesel combustion. Thissuppression effect is exhibited mostly in the reduction of elemental carbon and largermolecular weight PAHs. Moreover, the particle compositions were found to be loadand size dependeent.(4) Roadside sampling was made immediately adjacent to a freeway in Shanghai. Particle
samples were collected during daytime and nighttime. The physicochemicalcharacteristics of particle samples were investigated including size-resolved particlemass concentration, morphology, composition. These results were compared withthose of background samples. The results indicated that the vehicle emissionscontributes mostly to the size range less than400nm, and the mass concentration ofelement carbon, nitrate and PAHs in the particles exhibits the most notable increase,when compared to the background. The source assignment method of positive matrixfactor was used to analyze the contribution ratio of different emission sources and theresults were used for the calculation of vehicle emission factor of different enginetypes. The results indicate that particle emission from diesel motor vehicles is themajor contributor of roadside particulate, especially for ultrafine particles with thecontribution ration above60%. In Shanghai, the emission factor of in-use diesel motorvehicles is still in a higher level in the comparison with some developed countries andregions.
（1）针对超低硫柴油、低硫柴油和生物柴油三种不同燃料，在台架实验条件下，采用基于数量和质量两种不同方法研究了压燃式发动机排气颗粒物挥发性及其粒径分布特征。研究表明，相对低硫柴油，燃用生物柴油可以有效降低发动机排气颗粒中挥发性成分的比排放率，然而相对超低硫柴油，燃用生物柴油所产生颗粒物中挥发性物质成分的比排放率有所增加，其挥发性物质成分主要集中在小尺寸颗粒物中。
（2）研究了不同发动机工况、不同动力学粒径、不同燃油条件下发动机排气颗粒物形态、内部纳米结构及氧化活性。研究发现，发动机颗粒物的氧化活性主要取决于颗粒物基本粒子尺寸、挥发性物质比例及内部纳米结构特征等。由于燃用生物柴油所产生颗粒物较小的基本粒子尺寸、较高的挥发性物质比例以及相对短小、扭曲的内部碳层结构，其在热重实验中表现出相对超低硫柴油、低硫柴油颗粒物更强的氧化活性，与此同时，颗粒物的基本粒子尺寸、挥发性及内部碳层结构又与缸内燃烧条件、动力学粒径有着密切的关系。
（3）通过台架实验，研究了不同发动机负荷、不同动力学粒径以及燃油特性对颗粒物主要成分的影响，成分研究内容主要包括有机碳、元素碳及16种多环芳烃。试验结果表明，燃用生物柴油对颗粒物排放的抑制效果主要表现在燃烧生成的成分，如元素碳、大分子量的多环芳烃等，同时颗粒物的主要成分亦存在着明显的负荷变化及粒径分布特征。
（4）选取了上海地区一条典型的高速公路，开展了机动车排气颗粒对大气环境影响的研究，分别考察了白天和晚上道路微环境下大气悬浮颗粒物的理化特性，并与背景样品做了对比，主要测试内容包括不同粒径颗粒物的形貌、质量浓度及所包含的有机碳、元素碳、水溶性离子及多环芳烃的质量浓度。实验发现机动车对环境颗粒物的影响主要集中在<400nm的粒径范围内，在颗粒物主要成分中，机动车排放对元素碳、硝酸盐及多环芳烃浓度的影响最为明显。基于台架实验所获得的柴油发动机的排放源特征，采用正交矩阵因子法对路边颗粒物样品的主要成分进行源解析研究，得出不同车型机动车（柴油车、汽油车）排放对路边大气颗粒物的贡献比例，并据此改进了基于燃油消耗机动车颗粒物排放因子的计算方法，得出了不同车型机动车排放因子。计算结果表明，柴油车颗粒物排放是道路微环境下大气悬浮颗粒物的最主要贡献者，尤其对超细颗粒物的贡献达到60%以上。上海地区现行柴油车辆的颗粒物排放因子相对一些发达国家和地区仍处于一个比较高的水平。
Increased level of atmospheric aerosol can severely impact atmosphere visibility, publichealth and climate. With the rapid increase of vehicles in China, particulate emission has beenbecome one of the most important pollutant sources for atmospheric aerosol. Acomprehensive knowledge on physicochemical characteristics of vehicle particulate emissionis required to understand particle formation mechanism, hazards to the atmosphereenvironment, source assignment and ways to reduce particulate emission from motor vehicles.In this dissertation work, detailed physicochemical characteristics of particulate emissionwere investigated by dynamometry and roadside sampling. For the roadside experiment, anew method was proposed to calculate the vehicle emission factor with different engine types.This thesis is composed of the following parts:
(1) In the dynamometer experiment, ultra low sulfur diesel fuel (ULSD, sulfur contentless than10ppm), biodiesel (BD) and low sulfur diesel fuel (LSD, sulfur content lessthan400ppm) were used as the fuels. Detailed physicochemical characteristicsincluding size-dependent particle volatility, particle morphology, nanostructure,oxidation property and major composition were investigated. The size-dependentvolatility was investigated on the basis of number and mass measurements. It wasfound that, the use of biodiesel could reduce the brake specific emission of volatilesubstance effectively in comparison with LSD. While volatile substances in thebiodiesel particulate are notably greater than ULSD particulates and moreconcentrated in the particulates with small size.
(2) Particle morphology, nanostructure and oxidation property were also investigated overranges of engine operation conditions, aerodynamic sizes, and fuel types. Theoxidation experiments suggest that the oxidation property of diesel particulate dependon the primary particle size, volatile fraction, and nanostructure. Due to the smallerprimary particle size, larger volatile content and greater disordered inner nanostructure,biodiesel particulate exhibite stronger tendenty to oxidation than those from ULSDand LSD. Moreover, in-cylinder combustion parameter and fuel properties control theprimary particle size, volatile content and inner nanostructure of diesel particles.
(3) Analysis of particle composition included organic carbon, element carbon andpolycyclic aromatic hydrocarbons. In this thesis, the effect of engine load,aerodynamic size and fuel type on particle composition were investigated. The use ofbiodiesel appears to reduce particulate emissions from diesel combustion. Thissuppression effect is exhibited mostly in the reduction of elemental carbon and largermolecular weight PAHs. Moreover, the particle compositions were found to be loadand size dependeent.(4) Roadside sampling was made immediately adjacent to a freeway in Shanghai. Particle
samples were collected during daytime and nighttime. The physicochemicalcharacteristics of particle samples were investigated including size-resolved particlemass concentration, morphology, composition. These results were compared withthose of background samples. The results indicated that the vehicle emissionscontributes mostly to the size range less than400nm, and the mass concentration ofelement carbon, nitrate and PAHs in the particles exhibits the most notable increase,when compared to the background. The source assignment method of positive matrixfactor was used to analyze the contribution ratio of different emission sources and theresults were used for the calculation of vehicle emission factor of different enginetypes. The results indicate that particle emission from diesel motor vehicles is themajor contributor of roadside particulate, especially for ultrafine particles with thecontribution ration above60%. In Shanghai, the emission factor of in-use diesel motorvehicles is still in a higher level in the comparison with some developed countries andregions.
引文
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