生物质燃烧颗粒物中有机质及源解析研究进展

对近年来有关生物质燃烧排放的颗粒物中有机化合物和有机示踪物的研究进展进行了综述,分析了各国学者根据有机示踪物研究城市大气颗粒物中生物质燃烧和其他排放源对空气污染的贡献,对以后的相关研究具有借鉴意义．     

北京一月大气气溶胶的化学成分及其谱分布

1983年1月分别在市中心生活区和市郊气象塔处进行了为期10天的气溶胶采样,获得26组分级采样样品,样品用PIXE方法进行了分析,得到了20种元素的浓度及其谱分布.发现大多数元素的谱分布都是双模的,但细粒和粗粒气溶胶分量的相对强度各不相同.Ca,Al和Ti等元素以粗粒态为主;Zn,As和Pb等以细粒态为主;Cl,K,S,Si等二种分量相当.其中S和Si的谱分布与过去文献中的报道有很大区别,表明它们来源的复杂性.粗粒态气溶胶中除个别元素外,城区浓度大约是市郊浓度的1.4倍,而细粒气溶胶各元素浓度城区与郊区差     

乌鲁木齐降水化学成分及来源分析

降水是大气中主要和次要污染物的重要收集器,是清除大气中颗粒物和气态污染物最好的清除剂。为了了解乌鲁木齐降水特征,本文利用离子色谱分析了2010年降水样品,研究表明,该区降水pH值在5.6~7.77之间,年均值为6.19,电导率变化范围为18.7~172.5μs·cm~(-1),年均值为57.73μs·cm~(-1)。降水中主要离子浓度排序为Ca~(2+)SO_4~(2-)NH_4~+Na~+Mg~(2+)Cl~-NO_3~-K~+F~-,Ca~(2+)是最主要的阳离子,SO2-4是最主要的阴离子,表明乌鲁木齐降水中的致酸物质主要是硫酸盐。总离子浓度季节变化特征表现为秋季高,冬季低。FA平均值为0.001,表明99.9%的降水酸度被碱性成分中和,NF计算结果表明Ca~(2+)具有很强的中和能力。从相关分析、富集因子来看,SO_4~(2-)和NO_3~-主要受人为源的控制,K+主要存在于土壤扬尘或生物质燃烧产生的细颗粒物中;Mg~(2+)主要来自陆源的土壤扬尘等;Cl~-主要来自海相输入,生物质燃烧、人类生活污水排放以及化工厂排放对Cl-也有很大贡献。     

华北典型农业区PM2.5组分分析与来源解析

华北大气污染区域化正在对农业生态区域产生显著影响,为了了解华北农业地区大气细颗粒物PM2.5的季节分布特征,2017年7月、9月、12月以及2018年4月在中国科学院禹城农业生态综合实验站进行分季节PM2.5样品采集,并测定分析了样品中31种化学成分.结果表明,碳质气溶胶总体的浓度水平为13.11±8.37μg m-3,有机碳(OC)冬春季节浓度较高,元素碳(EC)浓度在秋冬季节较高.同时OC/EC的比值在秋季明显偏低,表明在秋季二次碳质气溶胶对PM2.5贡献较小.水溶性离子浓度总体在冬季最高.NO3-/SO2-4比值在夏季明显偏低为0.69,华北地区夏季固定点源对大气污染的贡献相对较高.PM2.5中金属元素以Na、Mg、Al、Ca、K、Fe等地壳元素为主,具有致癌风险的Co、Cr、Ni、Pb、As等金属元素年均浓度为0.32±0.24 ng m-3、5.40±5.42 ng m-3、10.23±7.46 ng m-3、42.23±27.75 ng m-3、5.66±3.79 ng m-3.受体模型(PMF)计算结果表明,PM2.5的主要来源为二次污染源、生物质燃烧源、燃煤燃油源、柴油车尾气和土壤源,贡献率分别达37.1％、18.2％、14.2％、9.4％和7.9％,表明农业区细颗粒物污染受到华北工业、农业与自然排放的多重影响.     

秸秆燃烧排放对北京及其周边地区PM2.5浓度影响的数值模拟

采用卫星监测的火点燃烧排放数据,利用区域化学传输模式WRF-Chem模拟分析了2017年5月华北地区细颗粒物(PM2.5)质量浓度分布,通过生物质燃烧排放源(华北区域以秸秆燃烧为主)开关的敏感性试验定量计算了燃烧排放对北京及其周边地区PM2.5质量浓度的影响。卫星监测结果显示,2017年5月华北地区有大量的秸秆焚烧现象,对该地区空气质量造成一定影响的燃烧天数为20 d,占全月总日数的65%左右。数值模拟结果表明:该地区秸秆燃烧排放导致PM2.5浓度升高的区域集中在华北平原农作物产区,其分布位置与卫星监测的火点分布吻合。秸秆燃烧导致这些地区PM2.5浓度月平均值上升幅度普遍超过3 μg/m~3,高值区超过了11 μg/m~3,上升比例可达10%以上;此外,来自华北平原及长三角地区的燃烧排放对北京(特别是东南部地区)污染物浓度的影响是不容忽视的,其中河南、山东、天津等地的秸秆燃烧在合适风场的作用下会严重影响北京,可导致丰台及通州等地PM2.5小时浓度上升超过17 μg/m~3,上升幅度超过40%。     

西安市夏季空气颗粒物污染特征及来源分析

大气颗粒物一直是西安市的主要污染物,多年监测的TSP日均浓度值均超过国家二级标准限值150 μg/m3。1996年夏季在西安市南郊陕西省委党校设立监测点,使用步进式时间序列自动采样仪对当地空气颗粒物进行了4天24小时连续采样,使用PIXE对采到的32个样品进行元素分析,每个样品分析出14～16种元素。各种元素浓度随时间变化趋势基本一致,主要受气象条件的影响,降雨对空气颗粒物各元素浓度有明显抑制作用。富集因子分析表明,西安市空气颗粒物不仅受地壳物质的影响,还受到一定程度人为污染的影响。元素浓度的因子分析表明,西安市夏季颗粒物主要有4种来源：地壳物质、有色治炼、燃煤排放源和化工制药业。     

北京北郊冬季低空大气气溶胶分析

文章分析了2001年1月10～16日和2月20日～3月2日两时段北京北郊中国科学院大气物理研究所325 m高的气象塔上距地面320、100和8 m 3个高度所采得的气溶胶样品的物理化学特征.计算了气溶胶的TSP浓度、化学组分及其分布和粒度谱.探讨了气象条件对气溶胶浓度及其来源和分布的影响.初步发现在所测的高度范围内,气溶胶TSP的浓度随高度的增高而下降,70%以上浓度分布在细粒组(d<2.1 μm).气溶胶中浓度最高的前20个元素是S、Fe、Ca、Al、K、Na、Mg、Zn、P、Ti、Pb、Ba、Mn、Cu、V、As、Cr、 Rb、Sb和Br.挥发性元素主要分布在细粒组,元素浓度随高度增加而减少.气溶胶的离子浓度也有相同的分布特征.风速变小、层结呈现稳定,尤其逆温以及大气湿度升高均为气溶胶浓度升高的因素.人为排放源是大气气溶胶的主要贡献者.导致北京严重空气污染的气溶胶源地以北京当地及其周边邻近地区的污染源为主.     

武汉市源成分谱特征研究

通过采集武汉市土壤风沙尘、建筑水泥尘、城市扬尘、餐饮源、生物质燃烧源、工业煤烟尘和电厂煤烟尘等7类源样品,并分析其碳组分、水溶性离子组分和无机元素组分,建立PM₁₀和PM_2.5源成分谱.研究表明,地壳元素Si、Ca、Al以及Fe等是土壤风沙尘的主要特征组分,其中Si是含量最高的成分,也是土壤风沙尘的标识组分.无组织建筑水泥尘中Si和Ca元素含量较高,将Ca元素作为无组织建筑水泥尘区别其他源类的重要元素,而有组织建筑水泥尘中OC、SO₄^2-含量比无组织建筑水泥尘高.城市扬尘中Ca的含量相对较高,表明城市扬尘受到建筑水泥尘影响较多.生物质燃烧源成分谱中OC的含量远高于成分谱中其他组分,另外Cl^-和K的平均含量也较高,K一般为生物质源的特征元素.     

南京北郊气溶胶中多环芳烃的污染特征及来源解析

利用2010年8月采集的南京北郊气溶胶样品,使用GC-MS对美国环保总局推荐的16种优先控制的多环芳烃含量、分布特征进行了研究。在此基础上,用特征比值法、主因子分析法分析得到南京市北郊大气中PAHs的主要来源为车辆尾气、燃煤、天然气和草木秸秆燃烧,并应用绝对因子分析法进一步定量计算主要源对PAHs的浓度贡献率。结果表明:1)大气颗粒物中16种多环芳烃的平均总质量浓度为135.85 ng/m~3,多环芳烃以4环为主,在可吸入颗粒物中的浓度占总浓度的88.7%;2)PM10中多环芳烃呈双模态分布,在9~10μm的粗模态和0.65~1.10μm的积聚模态上各出现一个峰值;3)天然气等对PAHs的贡献率为5.7%~44.1%,燃煤源的贡献率为20.7%~57.8%,汽车尾气的贡献率为4.6%~46.7%,木材燃烧的贡献率为2.9%~38.1%。本地交通排放和燃料燃烧是南京北郊大气颗粒物中PAHs的主要来源,远距离输送也对南京北郊气溶胶中的PAHs有重要贡献。     

东南亚生物质燃烧对我国霾和降水的影响

基于生物质燃烧排放源清单、地面观测和数值模式对东南亚中南半岛生物质燃烧气溶胶的排放特征,以及其在2020年春季对我国云南地区霾天气和南方前汛期降水过程的影响进行了分析.结果 表明:中南半岛生物质燃烧气溶胶排放主要集中于每年3-4月,排放峰值时段集中于3月下旬至4月上旬,主要排放区域为缅甸东部和老挝北部.中南半岛生物质燃...     

秸秆燃烧对北京秋季气溶胶浓度和短波辐射影响的模拟研究

利用地面细颗粒物（PM2.5）浓度和气象常规观测资料、地基 AERONET观测资料、GFED生物质燃烧排放清单和大气化学—天气耦合模式WRF-Chem,模拟研究了华北地区2014年10月气象要素和大气污染物的时空演变,重点关注北京10月7～11日的一次重霾事件及其天气形势、边界层气象特征、输送路径、PM2.5及其化学成分浓度变化等特征,以及秸秆燃烧对华北和北京地区细颗粒物浓度和地面短波辐射的影响。与观测资料的对比结果显示,模式可以很好地模拟北京地区地面气象要素和PM2.5质量浓度,考虑秸秆燃烧排放源可以明显改进北京PM2.5浓度模拟的准确性,但在重度污染情况下,模式总体上低估气溶胶光学厚度和高估地面短波辐射。10月7～11日北京地区重霾事件主要是不利气象条件下人为污染物累积和区域输送造成,也受到华北地区南部秸秆燃烧的影响。河南北部、河北南部和山东西部大面积秸秆燃烧释放的气态污染物和颗粒物在南风的作用下输送至北京,秸秆燃烧对北京地区地面PM2.5、有机碳（OC）、硝酸盐、铵盐、硫酸盐和黑碳（BC）的平均贡献率分别为24.6%、36.8%、23.2%、22.6%、7.1%和19.8%,秸秆燃烧产生的气溶胶可以导致北京地面平均短波辐射最大减小超过20 W m－2,约占总气溶胶导致地表短波辐射变化的24%。     

A comparison analysis of chemical composition of aerosols in the dust and non-dust periods in Beijing

Dust events occurred frequently in Beijing in recent years. In this work, 120 aerosol samples werecollected in two typical dust events (21-22 March and 15 May) and a non-dust period in Beijing fromMarch to May 2001. Samples were analyzed for major elemental components by the Proton Induced X-ray Emission (PIXE) method. Results show that the enrichment factors of crustal elements such as Mg,A1, and Ti had little differences between the dust period and the non-dust period in Beijing, while theenrichment factors of other elements that have a relation to anthropogenic emissions were very low duringthe dust period. The results derived by using multivariate factor analysis from the observation data showthat the sources such as soil dust, industry, and fuel combustion were among the major contributors tothe particles in Beijing.     

Roadside, Urban, and Rural comparison of size distribution characteristics of PAHs and carbonaceous components of Beijing, China

Size-segregated aerosol samples were collected with a low-pressure impactor (LPI) at urban, roadside and rural sites in winter in Beijing. The size distribution of Polycyclic Aromatic Hydrocarbons (PAHs), organic carbon (OC) and elemental carbon (EC) were measured and this study focused on their size distributions and relationships of PAH to OC/EC. All PAHs show uni-modal at the accumulation mode (0.1–1.8 μm) and almost all PAHs are associated with fine particles. The absence of PAHs in the nucleus mode contributes to the coagulation under the condition of high concentration of the accumulation mode particles. The absence of PAHs in the coarse mode was probably attributed to the low temperature that restrained the redistribution of PAHs from the accumulation mode to the coarse mode. Flu(fluoranthene) and Pyr(pyrene, 4-ring) were the most abundant particulate PAHs ; however, IcdP(indeno[1,2,3-cd]pyrene) and BghiP(benzo[ghi]perylene, 6-ring) were rather low. Diagnostic ratios show vehicle and coal burning were the major sources of PAHs in winter. Ratios at rural site are obviously different from those found at roadside and urban sites. Lower value of OC/EC in the rural area than that in the urban area was probably resulted from coal burning prevailed in the rural area. OC1 and OC2 exhibit uni-mode distribution similar to their particle surface area distribution indicating their existence on particles by adsorption. OC3 and OC4 show bi-mode distribution. Grinding of biomass debris can be a probable source of OC3 and OC4 in the coarse mode. EC1 is mostly from the pyrolysis of OC; however, both the natural and anthropogenic emissions contribute to EC2. The correlation between size-segregated PAHs and carbonaceous component is also discussed to identify their sources.     

Chemical composition of PM2.5 at an urban site of Chengdu in southwestern China

PM2.5 aerosols were sampled in urban Chengdu from April 2009 to January 2010, and their chemical compositions were characterized in detail for elements, water soluble inorganic ions, and carbonaceous matter. The annual average of PM2.5 was 165g m－3, which is generally higher than measurements in other Chinese cities, suggesting serious particulate pollution issues in the city. Water soluble ions contributed 43.5% to the annual total PM2.5 mass, carbonaceous aerosols including elemental carbon and organic carbon contributed 32.0%, and trace elements contributed 13.8%. Distinct daily and seasonal variations were observed in the mass concentrations of PM2.5 and its components, reflecting the seasonal variations of different anthropogenic and natural sources. Weakly acidic to neutral particles were found for PM2.5. Major sources of PM2.5 identified from source apportionment analysis included coal combustion, traffic exhaust, biomass burning, soil dust, and construction dust emissions. The low nitrate: sulfate ratio suggested that stationary emissions were more important than vehicle emissions. The reconstructed masses of ammonium sulfate, ammonium nitrate, particulate carbonaceous matter, and fine soil accounted for 79% of the total measured PM2.5 mass; they also accounted for 92% of the total measured particle scattering.     

Occurrence of water soluble organic nitrogen in aerosols at a coastal area

Aerosol samples (205) were collected from January 2005 to November 2006 at a coastal site at Keelung City (Taiwan), on the southern East China Sea. The atmospheric concentrations of major ions indicated that the area was dominated by different air masses at different times of the year: continental Asia from January to May and November to December; air masses from Indonesia and surrounding islands (south-eastern region) dominated during early-summer (July 2005 and June 2006), and air masses directly from the adjacent ocean dominated during late-summer (July to August 2006) and early-autumn (September to October 2005). The atmospheric concentrations of water soluble organic nitrogen (WSON) corresponded to the different sources and weather conditions. The results of a factor analysis of combined major ions, water soluble inorganic nitrogen (WSIN) and WSON indicated that a fossil fuel combustion source and biomass burning were the two major controlling factors during the sampling period. We discuss the correlations between WSON, WSIN and major anthropogenic ions in relation to the different formation mechanisms for the various sources. We propose a mechanism whereby biomass burning is the major input of aerosols derived from mainland China. Fossil fuel combustion was found to be important during periods when aerosols were derived from the south-eastern area. Our data indicate that WSON was predominantly associated with aerosols derived from biomass burning when the origin of the air mass was mainland China.     

The sources and seasonal variations of organic compounds in PM<Subscript>2.5</Subscript> in Beijing and Shanghai

Fine aerosol samples were collected throughout spring, summer, and winter in 2004∼2005 at a major urban traffic junction (BNU) and a suburban location (MY) in Beijing and at a downtown site (SH) in Shanghai, China. Ten of the 16 EPA priority polycyclic aromatic hydrocarbons (PAHs), seven fatty acids, levoglucosan, and cholesterol were identified and quantified. PAHs detected in Beijing and Shanghai were up to one order of magnitude higher than those reported in the developed countries either in urban or suburban areas, while levoglucosan was one order of magnitude lower than that in other countries for no biomass combustion in domestic heating in the mega-cities in China. PAHs showed the same seasonal trend in all sampling sites as the highest in winter and the lowest in summer, while fatty acids no pronounced seasonal variation. A significant fraction of levoglucosan from cooking with higher concentrations in urban than in suburban area contributed to the ambient atmosphere, indicating that the main source of levoglucosan in urban environment would be cooking rather than biomass burning. The relative contributions of coal combustion and vehicle exhaust sources to PAHs in fine aerosols were preliminarily estimated to be 1:2 in Beijing and 1:1 in Shanghai, revealing that the air pollution in these mega-cities in China was mainly the mixing of coal combustion with vehicle exhaust. Cooking was one of the major sources of organic aerosols in both Beijing and Shanghai.     

Aging of savanna biomass burning aerosols: Consequences on their optical properties

During the FOS-DECAFE experiment at Lamto, Ivory Coast, in January 1991, various ground studies were undertaken simultaneously in order to investigate the physical and chemical characteristics of smoke emitted by savanna biomass burning. Here we present sunphotometer ground-based results which allow the measurements of the spectral optical depth between 450 and 850 nm, the atmospheric water vapour content and the particle size distribution spectrum. The carbonaceous content of the savanna biomass burning aerosols is also investigated. This is the first time that the physical characteristics of particles emitted by savanna plumes are obtained from ground-field studies. All the results suggest that a rapid aging of the smoke occurs first hundred metres from the savanna fire èmission source. They show a relationship between the optical properties of smoke and the chemical aging of the aerosols primarily due to particle growth and a loss of organic material relative to the black carbon content.     

Modification of sea-salt aerosols over the coastal area in china

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CALIOP对一次秸秆焚烧后气溶胶光学特性的探测分析

采用星载激光雷达(Cloud - Aerosol LIdar with Orthogonal Polarization,CALIOP)资料研究了2008年6月2日华东秸秆焚烧排放气溶胶的光学特性,并与2006～2008年统计结果进行了对比.结果表明:1)CALIOP能够有效探测到气溶胶层,探测结果符合生物质燃烧气溶胶的...     

2008年北京奥运会期间大气气溶胶物理特征分析

应用MODIS卫星的气溶胶产品资料和地面的光学粒子计数器的资料,对比分析了北京地区2006、2007、2008年7～9月的气溶胶光学厚度、细粒子光学厚度、Angstrom指数、气溶胶粒子数浓度谱及体积谱,发现2008年北京奥运会期间(7月20日～9月20日)的气溶胶光学厚度比2006、2007年同期明显降低,气溶胶细模态光学厚度占总光学厚度的比上升,Angstrom指数上升,气溶胶细粒子数浓度没有明显相对变化,而粗粒子数浓度则减少约50%.利用大气标高,将MODIS反演的气溶胶柱的质量浓度转化为地面气溶胶质量浓度.用粒子计数器得到的体积谱,在假定气溶胶粒子密度的情况下,计算出其质量浓度.将这两种方法得到的气溶胶质量浓度与国家环境保护部公布的空气质量指数换算得到的可吸入颗粒物(PM10)质量浓度进行比较.结果表明:北京奥运期间空气质量总体达到了国家二级空气质量标准;与2006、2007年同期相比,2008年气溶胶PM10质量浓度明显下降,而这主要是由气溶胶粗粒子的减少引起的.