大气气溶胶酸度的研究进展

大气气溶胶的环境效应、气候效应和健康效应均与气溶胶的物理化学性质直接相关,其中大气气溶胶酸度是其重要的性质之一。大气气溶胶酸度对酸沉降、灰霾的形成具有重要作用,并影响大气非均相化学反应,相关研究已成为国际研究的热点。对国内外学者近年来在大气气溶胶酸度对大气环境与人体健康的影响、大气气溶胶酸度的影响因素与变化规律、大气气溶胶酸度/酸化缓冲能力的测定与计算方法、大气气溶胶酸性成分采集系统等方面的研究进展作了较系统的综述,并对大气气溶胶酸度研究未来的发展进行了展望。     

含碳气溶胶研究进展：有机碳和元素碳

含碳气溶胶是我国大气区域性复合型污染的重要物种,对全球气候变化、辐射强迫、能见度、环境质量、人类健康等会产生重要影响.主要从含碳气溶胶来源及成因、环境影响、样品采集及测试等方面对国内外相关研究进行了评述,讨论了有机碳和元素碳研究中存在的关键和难点问题,并对其发展前景进行了展望.     

大气气溶胶含碳物质基本特征综述

准确界定了气溶胶含碳物质,特别是有机碳和元素碳的基本概念,指出了元素碳与黑碳的异同,总结了有机碳和元素碳的排放源,以及二次有机碳的经验公式.阐述了有机碳、元素碳对全球气候、大气化学过程及人体健康带来的危害及机理.归纳了气溶胶中有机碳、元素碳组分的空间分布特征、时间变化特征.概述了国内气溶胶有机碳、元素碳的研究状况,指出国内相关研究重点和趋势.     

南京市大气气溶胶中颗粒物和正构烷烃特征及来源分析

于2002年夏季（7月）和冬季（12月）采集南京市5个功能区的大气气溶胶（PM2．5和PM10）样品，对两个季节不同功能区颗粒物及其颗粒物中正构烷烃的分布特征和污染来源进行了分析。结果表明，南京市大气颗粒物含量冬季高于夏季，细颗粒高于粗颗粒。正构烷烃的变化规律同颗粒物一致，且主要分布在细颗粒物上。根据各个功能区正构烷烃（C15-C32）的CPI（CPI1、CPI2和CPI3）结果，可知南京市大气气溶胶中正构烷烃由生物源和人为源共同排放产生。％waxCn的结果表明生物源对气溶胶中正构烷烃的贡献率为20％～43％，对南京市大气颗粒物的贡献率为1．66％～4．76％。     

高压液相色谱法快速测定环境空气中ppb级醛类

前言 由于大气醛类和其他羰基化合物是气态碳氢化合物的光氧化产物,是污染大气中有机气溶胶和自由基的主要来源以及在形成光化学烟雾中所起的关键作用,醛的分析已引起世界各国的广泛注意.醛从工厂或机动车可直接排入大气.作为室内涂料的脲醛树脂和类似粘合剂能散发出甲醛,造成室内污     

杭州市区降水酸度的初步分析

一、引言近数十年来,很多地区的降水酸度明显增加,其主要原因是由于燃烧化石燃料产生了硫和氮的氧化物,形成了呈酸性的大气污染物气溶胶。这些气溶胶粒子和其它物质会以各种方式改变降水的 pH 值,如二氧化硫、硫化氢能局部改变降水的化学性质。氮的氧化物可以转     

含碳气溶胶采样偏差评估方法研究进展

含碳气溶胶采样偏差是影响含碳气溶胶及大气颗粒物精确测定的主要因素之一,进而影响大气颗粒物的源解析、环境效应分析、污染防治对策制定等。分析了含碳气溶胶采样偏差的产生原因,综述了目前研究所用的衡量采样偏差的方法,并分析了方法的优缺点,探讨了引起采样偏差的主要影响因素,最后对今后的相关研究方向进行了展望。     

石英舟皿热解2-氨基(口白)啶硫酸盐法测定雨、雪水中硫酸根

我国是以燃煤为主要能源的国家,硫的污染大部分是由于煤碳燃烧排放二氧化硫造成的,二氧化硫在大气的温度、湿度及光照条件经过复杂的化学反应,生成硫酸雾,硫酸盐等二次污染物质以气溶胶的形式滞留在大气中。而雨、雪水在形式与降落过程中又吸附、捕集大气中的各种污染物质,包括硫酸雾和硫酸盐,然后随雨水降落到地面,它使土壤、河水酸化,污染地面水质,对人类、     

大气气溶胶采样和化学分析技术

本文是中美合作研究大气气溶胶化学成分的一系列论文的第一篇。主要介绍两种便于野外操作的气溶胶采样仪器和七十年代发展起来的特别适用于气溶胶化学分析的一种化学分析法——质子激发X-射线发射分析法(简写为PIXE)。     

超高效气溶胶净化系统有效性现场检验研究

各类超高效气溶胶净化系统普遍存在的较为突出的问题是:缺乏系统工作有效性现场检测手段,难以判断系统防护是否失效。根据超高效滤料过滤特性和测试原理,并在分析了大气气溶胶对过滤效率测试影响的基础上,提出大气气溶胶背景下,基于粒数浓度测量和使用发生的高浓度单分散气溶胶作为实验气溶胶的净化系统防护有效性现场检验测试技术及系统组成,并进行了验证。     

Source apportionment of surfactants in marine aerosols at different locations along the Malacca Straits

This study aims to determine the source apportionment of surfactants in marine aerosols at two selected stations along the Malacca Straits. The aerosol samples were collected using a high volume sampler equipped with an impactor to separate coarse- and fine-mode aerosols. The concentrations of surfactants, as methylene blue active substance and disulphine blue active substance, were analysed using colorimetric method. Ion chromatography was employed to determine the ionic compositions. Principal component analysis combined with multiple linear regression was used to identify and quantify the sources of atmospheric surfactants. The results showed that the surfactants in tropical coastal environments are actively generated from natural and anthropogenic origins. Sea spray (generated from sea-surface microlayers) was found to be a major contributor to surfactants in both aerosol sizes. Meanwhile, the anthropogenic sources (motor vehicles/biomass burning) were predominant contributors to atmospheric surfactants in fine-mode aerosols.     

A review of biomarker compounds as source indicators and tracers for air pollution

An overview of the application of organic geochemistry to the analysis of organic matter on aerosol particles is presented here. This organic matter is analyzed as solvent extractable bitumen/ lipids by gas chromatography-mass spectrometry. The organic geochemical approach assesses the origin, the environmental history and the nature of secondary products of organic matter by using the data derived from specific molecular analyses. Evaluations of production and fluxes, with cross-correlations can thus be made by the application of the same separation and analytical procedures to samples from point source emissions and the ambient atmosphere. This will be illustrated here with typical examples from the ambient atmosphere (aerosol particles) and from emissions of biomass burning (smoke). Organic matter in aerosols is derived from two major sources and is admixed depending on the geographic relief of the air shed. These sources are biogenic detritus (e.g., plant wax, microbes, etc.) and anthropogenic particle emissions (e.g., oils, soot, synthetics, etc.). Both biogenic detritus and some of the anthropogenic particle emissions contain organic materials which have unique and distinguishable compound distribution patterns (C₁₄-C₄₀). Microbial and vascular plant lipids are the dominant biogenic residues and petroleum hydrocarbons, with lesser amounts of the pyrogenic polynuclear aromatic hydrocarbons (PAH) and synthetics (e.g., chlorinated compounds), are the major anthropogenic residues. Biomass combustion is another important primary source of particles injected into the global atmosphere. It contributes many trace substances which are reactants in atmospheric chemistry and soot paniculate matter with adsorbed biomarker compounds, most of which are unknown chemical structures. The injection of natural product organic compounds into smoke occurs primarily by direct volatilization/steam stripping and by thermal alteration based on combustion temperature. Although the molecular composition of organic matter in smoke particles is highly variable, the molecular tracers are generally still source specific. Retene has been utilized as a tracer for conifer smoke in urban aerosols, but is not always detectable. Dehydroabietic acid is generally more concentrated in the atmosphere from the same emission sources. Degradation products from biopolymers (e.g., levoglucosan from cellulose) are also excellent tracers. An overview of the biomarker compositions of biomass smoke types is presented here. Defining additional tracers of thermally-altered and directly-emitted natural products in smoke aids the assessment of the organic matter type and input from biomass combustion to aerosols. The precursor to product approach of compound characterization by organic geochemistry can be applied successfully to provide tracers for studying the chemistry and dispersion of ambient aerosols and smoke plumes. Presented at the 6th FECS Conference on Chemistry and the Environment, Atmospheric Chemistry and Air Pollution, August 26–28, 1998, Copenhagen.     

Role of ammonia chemistry and coarse mode aerosols in global climatological inorganic aerosol distributions

We use an inorganic aerosol thermodynamic equilibrium model in a three-dimensional chemical transport model to understand the roles of ammonia chemistry and natural aerosols on the global distribution of aerosols. The thermodynamic equilibrium model partitions gas-phase precursors among modeled aerosol species self-consistently with ambient relative humidity and natural and anthropogenic aerosol emissions during the 1990s.Model simulations show that accounting for aerosol inorganic thermodynamic equilibrium, ammonia chemistry and dust and sea-salt aerosols improve agreement with observed SO₄, NO₃, and NH₄ aerosols especially at North American sites. This study shows that the presence of sea salt, dust aerosol and ammonia chemistry significantly increases sulfate over polluted continental regions. In all regions and seasons, representation of ammonia chemistry is required to obtain reasonable agreement between modeled and observed sulfate and nitrate concentrations. Observed and modeled correlations of sulfate and nitrate with ammonium confirm that the sulfate and nitrate are strongly coupled with ammonium. SO₄ concentrations over East China peak in winter, while North American SO₄ peaks in summer. Seasonal variations of NO₃ and SO₄ are the same in East China. In North America, the seasonal variation is much stronger for NO₃ than SO₄ and peaks in winter.Natural sea salt and dust aerosol significantly alter the regional distributions of other aerosols in three main ways. First, they increase sulfate formation by 10–70% in polluted areas. Second, they increase modeled nitrate over oceans and reduce nitrate over Northern hemisphere continents. Third, they reduce ammonium formation over oceans and increase ammonium over Northern Hemisphere continents. Comparisons of SO₄, NO₃ and NH₄ deposition between pre-industrial, present, and year 2100 scenarios show that the present NO₃ and NH₄ deposition are twice pre-industrial deposition and present SO₄ deposition is almost five times pre-industrial deposition.     

Seasonal variation and sources of carbonaceous species and elements in PM2.5 and PM10 over the eastern Himalaya

Environmental Science and Pollution Research - The study represents the seasonal characteristics (carbonaceous aerosols and elements) and the contribution of prominent sources of PM2.5 and PM10 in...     

Time-resolved measurements of aerosol elemental concentrations in indoor working environments

We have measured the elemental concentrations in aerosols with a 2-h time resolution in two different types of working environment: a chemistry laboratory dealing with the processing of advanced nanoparticulate materials and a medium-sized machine workshop. Non-stop 10-day and 12-day samplings were performed at each location in order to determine the concentration trends during the non-working/working and weekday/weekend periods. Supplementary measurements of PM10 aerosols with a 2-day sample collection time were performed with a standard Gent PM10 sampler to compare the elemental concentrations with the time-averaged concentrations detected by the 2D step-sampler. The concentrations were determined a posteriori by analyzing the x-ray spectra of aerosol samples emitted after 3-MeV proton bombardment. The PM10 samples collected in the chemistry laboratory were additionally inspected by scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDX) to determine the chemical compositions of the individual particles. In the workshop, a total PM10 mass sampling was performed simultaneously with a minute resolution to compare the signal with typical outdoor PM10 concentration levels. A factor analysis of the time-resolved dataset points to six and eight factors in the chemistry laboratory and the machine workshop, respectively. These factors describe most of the data variance, and their composition in terms of different elements can be related to specific indoor activities and conditions. We were able to demonstrate that the elemental concentration sampling with hourly resolution is an excellent tool for studying the indoor air pollution. While sampling the total PM10 mass concentration with a minute resolution may lack the potential to identify the emission sources in a “noisy” environment, the time averaging on a day time scale is too coarse to cope with the working dynamics, even if elemental sensitivity is an option.     

Sensitivity of urban ozone formation to chlorine emission estimates

Recent evidence has demonstrated that chlorine radical chemistry can enhance tropospheric volatile organic compound oxidation and has the potential to enhance ozone formation in urban areas. In order to investigate the regional impacts of chlorine chemistry in southeastern Texas, preliminary estimates of atmospheric releases of atomic chlorine precursors from industrial point sources, cooling towers, water and wastewater treatment, swimming pools, tap water, reactions of chlorides in sea salt aerosols, and reactions of chlorinated organics were developed. To assess the potential implications of these estimated emissions on urban ozone formation, a series of photochemical modeling studies was conducted to examine the spatial and temporal sensitivity of ozone and a unique marker species for chlorine chemistry, 1-Chloro-3-methyl-3-butene-2-one (CMBO), to molecular chlorine emissions estimates. Based on current estimates of molecular chlorine emissions in southeastern Texas, chlorine chemistry has the potential to enhance ozone mixing ratios by up to 11–16 ppbv. Impacts varied temporally, with emissions from cooling towers primarily responsible for a morning enhancement in ozone mixing ratios and emissions from residential swimming pools for an afternoon enhancement. Maximum enhancement in CMBO mixing ratios ranged from 59 to 69 pptv.     

Source apportionment of urban fine and ultra-fine particle number concentration in a Western Mediterranean city

Extensive measurements on particle number concentration and size distribution (13–800 nm), together with detailed chemical composition of PM_2.5 have constituted the main inputs of the database used for a source apportionment analysis. Data were collected at an urban background site in Barcelona, Western Mediterranean.The source identification analysis helped us to distinguish five emission sources (vehicle exhausts, mineral dust, sea spray, industrial source and fuel-oil combustion) and two atmospheric processes (photochemical induced nucleation and regional/urban background particles derived from coagulation and condensation processes). After that, a multilinear regression analysis was applied in order to quantify the contribution of each factor.This study reveals that vehicle exhausts contribute dominantly to the number concentration in all the particle sizes (52–86%), but especially in the range 30–200 nm. This work also points out the importance of the regional and/or urban formed aerosols (secondary inorganic particles) on the total number concentration (around 25% of the total number), with a higher impact on the accumulation mode. The photo-chemically induced nucleation of aerosols only represents a small proportion of the total number as an annual mean (3%), but is very relevant when considering only the nucleation mode (13–20 nm) fraction (23%). The other sources recognized registered sporadic contributions to the total number, coinciding with specific meteorological scenarios.This study discloses the main sources and features affecting and controlling the fine and ultra-fine aerosols in a typical city in the Western Mediterranean coast. Whereas the road traffic appears to be the most important source of sub-micrometric aerosols, other sources may not be negligible under specific meteorological conditions.     

Free amino acids in marine aerosols over the western North Pacific Ocean

Atmospheric input of fixed nitrogen species to the ocean has attracted considerable attention from the viewpoint of the oceanic biogeochemical cycle of nitrogen, although few measurements of organic nitrogen compounds in atmospheric aerosols have been extensively conducted over remote ocean areas. In this study, we report the geographical distribution of dissolved free amino acids (DFAA) in the water-soluble fraction of two size-segregated marine aerosols over the western North Pacific. The concentrations of DFAA showed higher values over the region north of 30°N, whereas they clearly decreased south of 30°N. Approximately 59–96% of DFAA was found in fine-mode particles. Long-range transport from continental sources could largely contribute to DFAA in marine aerosols over the remote North Pacific.     

Physicochemical variations in atmospheric aerosols recorded at sea onboard the Atlantic–Mediterranean 2008 Scholar Ship cruise (Part II): Natural versus anthropogenic influences revealed by PM10 trace element geochemistry

The geochemistry of PM₁₀ filter samples collected at sea during the Scholar Ship Atlantic–Mediterranean 2008 research cruise reveals a constantly changing compositional mix of pollutants into the marine atmosphere. Source apportionment modelling using Positive Matrix Factorization identifies North African desert dust, sea spray, secondary inorganic aerosols, metalliferous carbon, and V–Ni-bearing combustion particles as the main PM₁₀ factors/sources. The least contaminated samples show an upper continental crust composition (UCC)-normalised geochemistry influenced by seawater chemistry, with marked depletions in Rb, Th and the lighter lanthanoid elements, whereas the arrival of desert dust intrusions imposes a more upper crustal signature enriched in “geological” elements such as Si, Al, Ti, Rb, Li and Sc. Superimposed on these natural background aerosol loadings are anthropogenic metal aerosols (e.g. Cu, Zn, Pb, V, and Mn) which allow identification of pollution sources such as fossil fuel combustion, biomass burning, metalliferous industries, and urban–industrial ports. A particularly sensitive tracer is La/Ce, which rises in response to contamination from coastal FCC oil refineries. The Scholar Ship database allows us to recognise seaborne pollution sourced from NW Africa, the Cape Verde and Canary islands, and European cities and industrial complexes, plumes which in extreme cases can produce a downwind deterioration in marine air quality comparable to that seen in many cities, and can persist hundreds of kilometres from land.     

Precipitation chemistry in the coast of the Metropolitan Region of Rio de Janeiro, Brazil

Precipitation chemistry was studied in the Metropolitan Region of Rio de Janeiro (MRRJ). This study reveals that rainwater in the MRRJ is affected by emissions of air pollutants and provides essential data for future estimates of regional biogeochemical cycles and the impacts of acid deposition on tropical ecosystems. The volume-weighted mean (VWM) pH was 4.77, varying from 3.50 to 6.85. Sea-salt aerosols were the dominant sources of the Na+, Cl- and Mg2+. Excess SO4(2-), Ca2+ and K+ comprised 82, 91, and 87% of their total VWM concentrations, respectively. There were very strong correlations (r > 0.75, P > 0.01) for NO3- and H+, NO3- and excess(exc-)SO4(2-), NH4+ and exc-K+, and exc-SO4(2-) and exc-Ca2+, suggesting causal relationships between these ion pairs. The VWM concentrations of all major ions, except H+, were higher in the dry season, with dry to wet VWM concentration ratios varying from 1.1 (NH4+) to 4.7 (for total K+).