Assessment of natural components of PM10 at UK urban and rural sites

Proposals from the European Commission have raised the possibility that Member States may be able to subtract the concentrations of natural components of airborne particulate matter from measured concentrations when evaluating compliance with EU Limit Values. By applying the pragmatic mass closure model [Harrison et al., 2003. A pragmatic mass closure model for airborne particulate matter at urban background and roadside sites. Atmospheric Environment 37, 4927–4933] to chemical composition data for PM₁₀, it has been possible to estimate the concentrations of natural sea salt, strongly bound water and secondary organic carbon (which is assumed wholly biogenic) to the measured mass of PM₁₀. Because of the difficulty in distinguishing between natural and anthropogenic crustal dusts, the contribution of natural windblown dust and soil has not been accounted for. When the natural components are estimated for two urban and one rural site in the UK, the long-term mean PM₁₀ concentration is reduced by between 5.2 and 7.3 μg m⁻³. The number of exceedences of the 50 μg m⁻³ 24-h limit value falls dramatically from 54 to 21 (from a total of 291 days) at an urban street canyon site, 7 to 3 (n=292 days) at an urban background site and from 8 to 0 (n=241 days) at a rural site when using gravimetric PM₁₀ concentrations. The calculations have also been performed using PM₁₀ concentrations measured by TEOM increased by a factor of 1.3 as recommended by the European Commission as an interim means of estimating gravimetric equivalency, and the number of exceedences of the 24-h limit value fell from 92 to 47 (from a total of 291 days) at the urban street canyon site, from 11 to 3 (n=292 days) at the urban background site and from 6 to 3 (n=241) at the rural site. Clearly, therefore, application of this proposed measure would make a very major difference to the likelihood of compliance or otherwise with the 24-h limit value for PM₁₀.     

Sources and processes affecting concentrations of PM10 and PM2.5 particulate matter in Birmingham (U.K.)

Hourly average concentrations of PM₁₀ and PM_2.5 have been measured simultaneously at a site within Birmingham U.K. between October 1994 and October 1995. Comparison of PM₁₀ and NO_x data with two other sites in the same city shows comparable summer and winter mean concentrations and highly significant inter-site correlations for both hourly and daily mean data. Over a four-month period samples were also collected for chemical analysis of sulphate, nitrate, chloride, ammonium and elemental and organic carbon. Analysis of the data indicates a marked difference between summer and winter periods. In the winter months PM_2.5 comprises about 80% of PM₁₀ and is strongly correlated with NO_x indicating the importance of road traffic as a source. In the summer months, coarse particles (PM₁₀−PM_2.5) account for almost 50% of PM₁₀ and the influence of resuspended surface dusts and soils and of secondary particulate matter is evident. The chemical analysis data are also consistent with three sources dominating the PM₁₀ composition: vehicle exhaust emissions, secondary ammonium salts and resuspended surface dusts. Coarse particles from resuspension showed a positive dependence on windspeed, whilst elemental carbon derived from road traffic exhibited a negative dependence.     

Estimating uncertainties and uncertainty contributors of CMB PM2.5 source apportionment results

The chemical mass balance (CMB) model was applied for source apportionment of PM_2.5 in Atlanta in order to explore levels and causes of uncertainties in source contributions. Monte Carlo analysis with Latin hypercube sampling (MC-LHS) was performed to evaluate the source impact uncertainties and quantify how uncertainties in ambient measurement and source profile data affect results. In general, uncertainties in the source profile data contribute more to the final uncertainties in source apportionment results than do those in ambient measurement data. Uncertainty contribution estimates suggest that non-linear interactions among source profiles also affect the final uncertainties although their influence is typically less than uncertainties in source profile data.     

The impact of wood smoke on ambient PM2.5 in northern Rocky Mountain valley communities

During the winters of 2006/2007 and 2007/2008, PM_2.5 source apportionment programs were carried out within five western Montana valley communities. Filter samples were analyzed for mass and chemical composition. Information was utilized in a Chemical Mass Balance (CMB) computer model to apportion the sources of PM_2.5. Results showed that wood smoke (likely residential woodstoves) was the major source of PM_2.5 in each of the communities, contributing from 56% to 77% of the measured wintertime PM_2.5. Results of ¹⁴C analyses showed that between 44% and 76% of the measured PM_2.5 came from a new carbon (wood smoke) source, confirming the results of the CMB modeling. In summary, the CMB model results, coupled with the ¹⁴C results, support that wood smoke is the major contributor to the overall PM_2.5 mass in these rural, northern Rocky Mountain airsheds throughout the winter months.     

PM2.5 chemical source profiles for vehicle exhaust, vegetative burning, geological material, and coal burning in Northwestern Colorado during 1995

PM_2.5 (particles with aerodynamic diameters less than 2.5 μm) chemical source profiles applicable to speciated emissions inventories and receptor model source apportionment are reported for geological material, motor vehicle exhaust, residential coal (RCC) and wood combustion (RWC), forest fires, geothermal hot springs; and coal-fired power generation units from northwestern Colorado during 1995. Fuels and combustion conditions are similar to those of other communities of the inland western US. Coal-fired power station profiles differed substantially between different units using similar coals, with the major difference being lack of selenium in emissions from the only unit that was equipped with a dry limestone sulfur dioxide (SO₂) scrubber. SO₂ abundances relative to fine particle mass emissions in power plant emissions were seven to nine times higher than hydrogen sulfide (H₂S) abundances from geothermal springs, and one to two orders of magnitude higher than SO₂ abundances in RCC emissions, implying that the SO₂ abundance is an important marker for primary particle contributions of non-aged coal-fired power station contributions. The sum of organic and elemental carbon ranged from 1% to 10% of fine particle mass in coal-fired power plant emissions, from 5% to 10% in geological material, >50% in forest fire emissions, >60% in RWC emissions, and >95% in RCC and vehicle exhaust emissions. Water-soluble potassium (K⁺) was most abundant in vegetative burning profiles. K⁺/K ratios ranged from 0.1 in geological material profiles to 0.9 in vegetative burning emissions, confirming previous observations that soluble potassium is a good marker for vegetative burning.     

Determination and analysis of PM10 source apportionment during episodes of air pollution in Central Eastern European urban areas: The case of wintertime 2006

Source apportionment of air pollution due to particulate matter with an aerodynamic diameter <10 μm (PM₁₀) was investigated in Central Eastern European urban areas. A combination of four methods was developed to distinguish long-range transport (LRT) and regional transport (RT) from local pollution (LP) sources as well as to discern the involvement of traffic or residential sources in LP. Sources of PM₁₀ events of pollution were determined in January 2006 in representative Polish cities using monitored air quality and meteorological data, backward air mass trajectories, correlation and principal component analysis (PCA). Daily patterns of PM₁₀ levels show that several peak episodes were registered in Poland; January 21–30th being the most polluted days. Air mass back-trajectory analysis shows that all cities were under the influence of LRT from North-eastern origins (Russia–Belarus–Ukraine), most were also under LRT from Southern origin (Slovakia, Czech Republic), and northern cities were under national RT influence. PCA analysis shows that ion-sums of secondary inorganic aerosols account for LRT pollution while arsenic and chromium represents markers of RT (industrial) and LP (residential) sources of PM₁₀, respectively. Determination of several ratios (REG/UB, REG/TRAF, TRAF/UB) calculated between PM₁₀ levels measured at regional background (REG); urban background (UB) and traffic (TRAF) monitoring sites shows that, with ratios REG/UB ≥ 0.57, PM₁₀ episodes in both Szczecin and Warsaw bore a marked RT origin. The lower REG/UB ≤ 0.35 in the Southern cities of Cracow and Zabrze indicates that LP was the main contributor to the observed episodes. Only PM₁₀ episodes in Southern-western Poland (Jelenia Góra) were clearly of LP origin as characterized, by the lowest REG/UB ratio (<0.2). The high TRAF/UB ratios obtained for all cities (close to 1) indicate that there was a great uniformity of PM levels on an urban scale owing to the meteorologically stagnant conditions. A high correlation between PM₁₀, NO₂ and CO confirms that traffic emission represented a common and an important LP source of urban pollution in most Polish cities during January 2006. On the other hand PM₁₀ which is also highly correlated with SO₂ in 4 cities out of 6, indicates that coal combustion through domestic heating or industrial activities was also an important LP source of PM₁₀. Finally, extremely unfavourable meteorological conditions caused by the influence of a Siberian high-pressure system were found to be associated with the occurrence of severe PM₁₀ episodes of pollution.     

Impact of the 1998 Central American fires on PM2.5 mass and composition in the southeastern United States

The impact of the Central American fires on PM_2.5 mass concentration and composition in the Tennessee Valley region during portions of May, 1998, has been quantified. Elevated concentrations of smoke aerosol tracers—fine potassium, (and to a lesser extent, calcium and silicon) and, where available, organic and elemental carbon—were observed in the region during times in which satellite imagery (TOMS and GOES-8) showed regional transport of hazy, smoky airmasses from southern Mexico and adjacent areas of Central America. Back-trajectories from network sites in the Tennessee Valley network were consistent with this regional transport. The extent of transport of extra-regional fine particle mass during May, 1998, is discussed relative to the new US fine particle mass-based standards for fine particulate matter.     

电除尘器电源交流分量对PM_(2.5)等细微颗粒物除尘效率的影响

除尘器对颗粒物的除尘效率与颗粒物的荷电量密切相关,PM2.5等细小颗粒物由于其荷电量不足而导致其吸收效率较低,对环境造成危害。为了增加粒子的荷电量,以粒子荷电原理为理论依据,从离子电流密度和通过电凝并扩大尘粒中位径2个方面研究了电除尘电源中交流电压分量对PM2.5等细小颗粒物荷电特性的影响,得出了电除尘器电源中交流电压分量可从以上2个方面提高装置对PM2.5等微小颗粒物的荷电量,且频率越高,幅值越大,荷电效果越好,从而可以提高装置对细小颗粒物的除尘效率。     

Characterization of carbonaceous species in PM2.5 in Xi'an during spring

The characterization of carbonaceous species in PM_2.5 during a spring period in a suburb of Xi'an, China was investigated. PM_2.5 samples were collected on quartz filters and analyzed for organic carbon (OC) and elemental carbon (EC). The thermal optical reflectance method was used. The minimum OC/EC ratio method was used to estimate the concentration of secondary organic carbon (SOC). The distribution of eight carbon fractions was investigated as well. The average mass concentrations of OC and EC were 15.90 and 8.38 μg/m³, respectively. The average OC/EC ratio ranged from 1.16 to 3.16 with an average value of 2.25. This implies the existence of SOC in PM_2.5. The mean SOC concentration was 7.20 μg/m³, accounting for 45.28% of total OC. This result suggests that SOC is a significant component of OC in the suburb of Xi'an. Results from the distribution of eight carbon fractions revealed that emissions from motor vehicle, coal combustion, and road dust were the main source of carbonaceous particles in the sampling period.     

The impacts of different kinds of dust events on PM10 pollution in northern China

In this study the frequencies of PM₁₀ (as key urban pollutant) in 14 key environmental protection cities in northern China were analyzed. It follows that the PM₁₀ concentration in the high-frequency period is higher with an extent 0.009–0.066 mg m⁻³ than in the low-frequency period of 2001–2002. Further the impacts of three kinds of dust events on the PM₁₀ concentration in four cities (Beijing, Hohhot, Xi’an and Lanzhou) were explored. The results showed that different kinds of dust events have different influences on variation of PM₁₀ concentration in these four cities. In Lanzhou and Hohhot, which are near the source areas of dust events, the contribution degree of these three dust events to the PM₁₀ is: floating dust>dust storm>blowing dust. Whereas, in Beijing and Xi’an situated in dust event passing areas, the mean value of PM₁₀ concentration is higher in blowing dust than in floating dust (no dust storm). In addition, the influences of dust events on PM₁₀ concentration are different in the cities on different dust event paths. In Beijing and Hohhot (on the northern path), the high PM₁₀ concentration is usually caused by blowing dust. But in both Lanzhou and Xi’an (on the western/northwestern path) the high PM₁₀ pollution concentration is usually caused by floating dust.     

Evaluation of the community multiscale air quality (CMAQ) model version 4.5: Sensitivities impacting model performance; Part II—particulate matter

This paper is Part II in a pair of papers that examines the results of the Community Multiscale Air Quality (CMAQ) model version 4.5 (v4.5) and discusses the potential explanations for the model performance characteristics seen. The focus of this paper is on fine particulate matter (PM_2.5) and its chemical composition. Improvements made to the dry deposition velocity and cloud treatment in CMAQ v4.5 addressing compensating errors in 36-km simulations improved particulate sulfate (SO₄²⁻) predictions. Large overpredictions of particulate nitrate (NO₃⁻) and ammonium (NH₄⁺) in the fall are likely due to a gross overestimation of seasonal ammonia (NH₃) emissions. Carbonaceous aerosol concentrations are substantially underpredicted during the late spring and summer months, most likely due, in part, to a lack of some secondary organic aerosol (SOA) formation pathways in the model. Comparisons of CMAQ PM_2.5 predictions with observed PM_2.5 mass show mixed seasonal performance. Spring and summer show the best overall performance, while performance in the winter and fall is relatively poor, with significant overpredictions of total PM_2.5 mass in those seasons. The model biases in PM_2.5 mass cannot be explained by summing the model biases for the major inorganic ions plus carbon. Errors in the prediction of other unspeciated PM_2.5 (PM_Other) are largely to blame for the errors in total PM_2.5 mass predictions, and efforts are underway to identify the cause of these errors.     

Seasonal variation and source estimation of organic compounds in urban aerosol of Augsburg, Germany

This study reports a general assessment of the organic composition of the PM_2.5 samples collected in the city of Augsburg, Germany in a summer (August-September 2007) and a winter (February-March 2008) campaign of 36 and 30 days, respectively. The samples were directly submitted to in-situ derivatisation thermal desorption gas chromatography coupled with time of flight mass spectrometry (IDTD-GC-TOFMS) to simultaneously determine the concentrations of many classes of molecular markers, such as n-alkanes, iso- and anteiso-alkanes, polycyclic aromatic hydrocarbons (PAHs), oxidized PAHs, n-alkanoic acids, alcohols, saccharides and others.The PCA analysis of the data identified the contributions of three emission sources, i.e., combustion sources, including fossil fuel emissions and biomass burning, vegetative detritus, and oxidized PAHs. The PM chemical composition shows seasonal trend: winter is characterized by high contribution of petroleum/wood combustion while the vegetative component and atmospheric photochemical reactions are predominant in the hot season.     

Regression modelling of hourly NOx and NO2 concentrations in urban air in London

Based on hourly measurements of NO_x NO₂ and O₃ and meteorological data, an ordinary least squares (OLS) model and a first-order autocorrelation (AR) model were developed to analyse the regression and prediction of NO_x and NO₂ concentrations in London. Primary emissions and wind speed are the most important factors influencing NO_x concentrations; in addition to these two, reaction of NO with O₃ is also a major factor influencing NO₂ concentrations. The AR model resulted in high correlation coefficients (R > 0.95) for the NO_x and NO₂ regression based on a whole year's data, and is capable of predicting NO₂ (R = 0.83) and NO_x (R = 0.65) concentrations when the explanatory variables were available. The analysis of the structure of regression models by Principal Component Analysis (PCA) indicates that the regression models are stable. The results of the OLS model indicate that there was an exceptional NO₂ source, other than primary emission and reaction of NO with O₃, in the air pollution episode in London in December 1991.     

Cocaine and other illicit drugs in airborne particulates in urban environments: a reflection of social conduct and population size

Levels of cocaine and other psychoactive substances in atmospheric particulate matter (PM) were determined in urban environments representing distinct social behaviours with regard to drug abuse: night-life, university and residential areas. Three cities (with population >1 million and <0.3 million inhabitants) were selected. Mean daily levels of drugs in PM were 11-336 pg/m³ for cocaine, 23-34 pg/m³ for cannabinoids, and 5-90 pg/m³ for heroin. The highest levels were recorded on weekends, with factors with respect to weekdays of 1-3 for cocaine, 1-2 for cannabinoids and 1.1-1.7 for heroin. Higher levels were detected in the night-life areas, pointing towards consumption and trafficking as major emission sources, and possibly ruling out drug manufacture. The similarities in temporal trends at all sites suggested a city-scale transport of psychoactive substances. Correlations were detected between cocaine and amphetamine consumption (r² = 0.98), and between heroin and cannabinoids (r²>0.82).     

Oxidative properties of ambient PM2.5 and elemental composition: Heterogeneous associations in 19 European cities

We assessed the extent to which constituents of PM_2.5 (transition metals, sodium, chloride) contribute to the ability to generate hydroxyl radicals (OH) in vitro in PM_2.5 sampled at 20 locations in 19 European centres participating in the European Community Respiratory Health Survey. PM_2.5 samples (n = 716) were collected on filters over one year and the oxidative activity of particle suspensions obtained from these filters was then assessed by measuring their ability to generate OH in the presence of hydrogen peroxide. Associations between OH formation and the studied PM constituents were heterogeneous. The total explained variance ranged from 85% in Norwich to only 6% in Albacete. Among the 20 centres, 15 showed positive correlations between one or more of the measured transition metals (copper, iron, manganese, lead, vanadium and titanium) and OH formation. In 9 of 20 centres OH formation was negatively associated with chloride, and in 3 centres with sodium. Across 19 European cities, elements which explained the largest variations in OH formation were chloride, iron and sodium.     

北京市交通道路空气中NO_x的污染现状及时空变化规律研究

基于2008年及2009年分4个季节对北京市3种类型道路(开阔型、交叉路口型和峡谷型)空气中的NOx的现场监测结果,分析了3种类型道路空气中NOx的污染现状和时空变化规律及影响因素。实验结果表明,昼间北京市各类型街道空气中NOx浓度呈早晚浓度高、中午浓度低的变化规律,NOx浓度随季节和车流量变化较明显。交通道路空气中NO占NOx的分担率高,且有较好的相关性,而NO2分担率较低,与NOx相关性较差。     

纳米TiO2/活性炭复合光催化剂的制备及其对甲醛气体降解

研究了纳米TiO2/活性炭复合光催化剂对空气中典型污染气体甲醛的光催化降解特性。采用扫描电镜(SEM)表征复合催化剂的表面特征。结果显示,经改性后的纳米TiO2在复合催化剂表面分布均匀,呈球状。对甲醛气体的降解实验显示TiO2负载量为1%时对甲醛的去除效果最好,6 h去除率为61.7%。结果显示复合催化剂把甲醛气体分解成CO2,可以直接排空,无二次污染。     

Diurnal changes in photosynthetic parameters of Populus tremuloides, modulated by elevated concentrations of CO2 and/or O3 and daily climatic variation

The diurnal changes in light-saturated photosynthesis (Pn) under elevated CO₂ and/or O₃ in relation to stomatal conductance (g_s), water potential, intercellular [CO₂], leaf temperature and vapour-pressure difference between leaf and air (VPD_L) were studied at the Aspen FACE site. Two aspen (Populus tremuloides Michx.) clones differing in their sensitivity to ozone were measured. The depression in Pn was found after 10:00 h. The midday decline in Pn corresponded with both decreased g_s and decreased Rubisco carboxylation efficiency, Vc_max. As a result of increasing VPD_L, g_s decreased. Elevated [CO₂] resulted in more pronounced midday decline in Pn compared to ambient concentrations. Moreover, this decline was more pronounced under combined treatment compared to elevated CO₂ treatment.The positive impact of CO₂ on Pn was relatively more pronounced in days with environmental stress but relatively less pronounced during midday depression. The negative impact of ozone tended to decrease in both cases.     

碳纳米管/二氧化钛/壳聚糖催化薄膜光催化活性及苯降解机理

通过X-射线衍射仪(XRD)、扫描电镜(SEM)、透射电镜(TEM)和紫外可见光漫反射谱(UV-vis)对碳纳米管/二氧化钛/壳聚糖复合薄膜的晶体结构和形貌进行表征,以室内空气典型污染物气相苯为模型反应物,研究碳纳米管/二氧化钛/壳聚糖催化薄膜的光催化活性及其对苯的光降解机理。结果表明,制备的碳纳米管/二氧化钛/壳聚糖催化薄膜所具有的良好催化活性归功于碳纳米管、二氧化钛和壳聚糖三者的协调效应;气相苯光降解产生的主要中间产物是乙酸乙酯和十一烷,以及少量的丙烯醛、4-羰基-甲基-苯乙酮、十二烷烃、2,4,-二叔丁基苯酚、二十一烷烃。根据红外光谱分析与GC/MS分析结果,进一步提出了气相苯的降解机理过程。     

Analysis of the relationship between ambient levels of O3, NO2 and NO as a function of NOx in the UK

Monitoring data from the UK Automatic Urban and Rural Network are used to investigate the relationships between ambient levels of ozone (O₃), nitric oxide (NO) and nitrogen dioxide (NO₂) as a function of NO_x, for levels ranging from those typical of UK rural sites to those observed at polluted urban kerbside sites. Particular emphasis is placed on establishing how the level of ‘oxidant’, OX (taken to be the sum of O₃ and NO₂) varies with the level of NO_x, and therefore to gain some insight into the atmospheric sources of OX, particularly at polluted urban locations. The analyses indicate that the level of OX at a given location is made up of NO_x-independent and NO_x-dependent contributions. The former is effectively a regional contribution which equates to the regional background O₃ level, whereas the latter is effectively a local contribution which correlates with the level of primary pollution. The local oxidant source has probable contributions from (i) direct NO₂ emissions, (ii) the thermal reaction of NO with O₂ at high NO_x, and (iii) common-source emission of species which promote NO to NO₂ conversion. The final category may include nitrous acid (HONO), which appears to be emitted directly in vehicle exhaust, and is potentially photolysed to generate HO_x radicals on a short timescale throughout the year at southern UK latitudes. The analyses also show that the local oxidant source has significant site-to-site variations, and possible reasons for these variations are discussed. Relationships between OX and NO_x, based on annual mean data, and fitted functions describing the relative contributions to OX made by NO₂ and O₃, are used to define expressions which describe the likely variation of annual mean NO₂ as a function of NO_x at 14 urban and suburban sites, and which can take account of possible changes in the regional background of O₃.