Brown Coal and Logwood Combustion in a Modern Heating Appliance: The Impact of Combustion Quality and Fuel on Organic Aerosol Composition.

Residential heating with solid fuels is one of the major drivers for poor air quality in Central and Eastern Europe, and coal is still one of the major fuels in countries, such as Poland, the Czech Republic, and Hungary. In this work, emissions from a single-room heater fueled with brown coal briquettes (BCBs) and spruce logs (SLs) were analyzed for signatures of inorganic as well as semivolatile aromatic and low-volatile organic constituents. High variations in organic carbon (OC) emissions of BCB emissions, ranging from 5 to 22 mg MJ-1, were associated to variations in carbon monoxide (CO) emissions, ranging from 900 to 1900 mg MJ-1. Residential BCB combustion turned out to be an equally important source of levoglucosan, an established biomass burning marker, as spruce logwood combustion, but showed distinct higher ratios to manosan and galactosan. Signatures of polycyclic aromatic hydrocarbons emitted by BCB combustion exhibited defunctionalization and desubstitution with increasing combustion quality. Lastly, the concept of island and archipelago structural motifs adapted from petroleomics is used to describe the fraction low-volatile organic compounds in particulate emissions, where a transition from archipelago to island motifs in relation with decreasing CO emissions was observed in BCB emissions, while emissions from SL combustion exhibited the island motif.

Spatiotemporal Characteristics and Driving Factors of Black Carbon in Augsburg, Germany: Combination of Mobile Monitoring and Street View Images.

The study investigates the spatial pattern of black carbon (BC) at a high spatial resolution in Augsburg, Germany. Sixty two walks were performed to assess the concentrations of equivalent black carbon (eBC), ultraviolet particulate matter (UVPM), and equivalent brown carbon (eBrC) in different seasons and at different times of the day with a mobile platform (i.e., trolley). Along with BC measurements, images of street microenvironments were recorded. Meteorological parameters, including temperature, relative humidity, and wind speed, were monitored. The BC concentrations showed significant spatial heterogeneity and diurnal variations peaking in the morning and at night. The highest BC concentrations were observed near dense traffic. The correlations between BC and street views (buildings, roads, cars, and vegetation) were weak but highly significant. Moreover, meteorological factors also influenced the BC concentration. A model based on street view images and meteorological data was developed to examine the driving factors of the spatial variability of BC concentrations at a higher spatial resolution as different microenvironments based on traffic density. The best results were obtained for UVPM and eBC (71 and 70% explained variability). eBrC (53%), to which other sources besides road traffic can also make significant contributions, is modeled less well.

High secondary aerosol contribution to particulate pollution during haze events in China.

Rapid industrialization and urbanization in developing countries has led to an increase in air pollution, along a similar trajectory to that previously experienced by the developed nations. In China, particulate pollution is a serious environmental problem that is influencing air quality, regional and global climates, and human health. In response to the extremely severe and persistent haze pollution experienced by about 800 million people during the first quarter of 2013 (refs 4, 5), the Chinese State Council announced its aim to reduce concentrations of PM2.5 (particulate matter with an aerodynamic diameter less than 2.5 micrometres) by up to 25 per cent relative to 2012 levels by 2017 (ref. 6). Such efforts however require elucidation of the factors governing the abundance and composition of PM2.5, which remain poorly constrained in China. Here we combine a comprehensive set of novel and state-of-the-art offline analytical approaches and statistical techniques to investigate the chemical nature and sources of particulate matter at urban locations in Beijing, Shanghai, Guangzhou and Xi'an during January 2013. We find that the severe haze pollution event was driven to a large extent by secondary aerosol formation, which contributed 30-77 per cent and 44-71 per cent (average for all four cities) of PM2.5 and of organic aerosol, respectively. On average, the contribution of secondary organic aerosol (SOA) and secondary inorganic aerosol (SIA) are found to be of similar importance (SOA/SIA ratios range from 0.6 to 1.4). Our results suggest that, in addition to mitigating primary particulate emissions, reducing the emissions of secondary aerosol precursors from, for example, fossil fuel combustion and biomass burning is likely to be important for controlling China's PM2.5 levels and for reducing the environmental, economic and health impacts resulting from particulate pollution.

Influence of wood species on toxicity of log-wood stove combustion aerosols: a parallel animal and air-liquid interface cell exposure study on spruce and pine smoke.

BACKGROUND: Wood combustion emissions have been studied previously either by in vitro or in vivo models using collected particles, yet most studies have neglected gaseous compounds. Furthermore, a more accurate and holistic view of the toxicity of aerosols can be gained with parallel in vitro and in vivo studies using direct exposure methods. Moreover, modern exposure techniques such as air-liquid interface (ALI) exposures enable better assessment of the toxicity of the applied aerosols than, for example, the previous state-of-the-art submerged cell exposure techniques. METHODS: We used three different ALI exposure systems in parallel to study the toxicological effects of spruce and pine combustion emissions in human alveolar epithelial (A549) and murine macrophage (RAW264.7) cell lines. A whole-body mouse inhalation system was also used to expose C57BL/6 J mice to aerosol emissions. Moreover, gaseous and particulate fractions were studied separately in one of the cell exposure systems. After exposure, the cells and animals were measured for various parameters of cytotoxicity, inflammation, genotoxicity, transcriptome and proteome. RESULTS: We found that diluted (1:15) exposure pine combustion emissions (PM1 mass 7.7 ± 6.5 mg m- 3, 41 mg MJ- 1) contained, on average, more PM and polycyclic aromatic hydrocarbons (PAHs) than spruce (PM1 mass 4.3 ± 5.1 mg m- 3, 26 mg MJ- 1) emissions, which instead showed a higher concentration of inorganic metals in the emission aerosol. Both A549 cells and mice exposed to these emissions showed low levels of inflammation but significantly increased genotoxicity. Gaseous emission compounds produced similar genotoxicity and a higher inflammatory response than the corresponding complete combustion emission in A549 cells. Systems biology approaches supported the findings, but we detected differing responses between in vivo and in vitro experiments. CONCLUSIONS: Comprehensive in vitro and in vivo exposure studies with emission characterization and systems biology approaches revealed further information on the effects of combustion aerosol toxicity than could be achieved with either method alone. Interestingly, in vitro and in vivo exposures showed the opposite order of the highest DNA damage. In vitro measurements also indicated that the gaseous fraction of emission aerosols may be more important in causing adverse toxicological effects. Combustion aerosols of different wood species result in mild but aerosol specific in vitro and in vivo effects.

Contributions of City-Specific Fine Particulate Matter (PM2.5) to Differential In Vitro Oxidative Stress and Toxicity Implications between Beijing and Guangzhou of China.

Growing literature has documented varying toxic potencies of source- or site-specific fine particulate matter (PM2.5), as opposed to the practice that treats particle toxicities as independent of composition given the incomplete understanding of the toxicity of the constituents. Quantifying component-specific contribution is the key to unlocking the geographical disparities of particle toxicity from a mixture perspective. In this study, we performed integrated mixture-toxicity experiments and modeling to quantify the contribution of metals and polycyclic aromatic hydrocarbons (PAHs), two default culprit component groups of PM2.5 toxicity, to in vitro oxidative stress caused by wintertime PM2.5 from Beijing and Guangzhou, two megacities in China. PM2.5 from Beijing exhibited greater toxic potencies at equal mass concentrations. The targeted chemical analysis revealed higher burden of metals and PAHs per unit mass of PM2.5 in Beijing. These chemicals together explained 38 and 24% on average of PM2.5-induced reactive oxygen species in Beijing and Guangzhou, respectively, while >60% of the effects remained to be resolved in terms of contributing chemicals. PAHs contributed approximately twice the share of the PM2.5 mixture effects as metals. Fe, Cu, and Mn were the dominant metals, constituting >80% of the metal-shared proportion of the PM2.5 effects. Dibenzo[ a, l]pyrene alone explained >65% of the PAH-shared proportion of the PM2.5 toxicity effects. The significant contribution from coal combustion and vehicular emissions in Beijing suggested the major source disparities of toxicologically active PAHs between the two cities. Our study provided novel quantitative insights into the role of varying toxic component profiles in shaping the differential toxic potencies of city-specific PM2.5 pollution.

Size-Resolved Identification, Characterization, and Quantification of Primary Biological Organic Aerosol at a European Rural Site.

Primary biological organic aerosols (PBOA) represent a major component of the coarse organic matter (OMCOARSE, aerodynamic diameter > 2.5 µm). Although this fraction affects human health and the climate, its quantification and chemical characterization currently remain elusive. We present the first quantification of the entire PBOACOARSE mass and its main sources by analyzing size-segregated filter samples collected during the summer and winter at the rural site of Payerne (Switzerland), representing a continental Europe background environment. The size-segregated water-soluble OM was analyzed by a newly developed offline aerosol mass spectrometric technique (AMS). Collected spectra were analyzed by three-dimensional positive matrix factorization (3D-PMF), showing that PBOA represented the main OMCOARSE source during summer and its contribution to PM10 was comparable to that of secondary organic aerosol. We found substantial cellulose contributions to OMCOARSE, which in combination with gas chromatography mass spectrometry molecular markers quantification, underlined the predominance of plant debris. Quantitative polymerase chain reaction (qPCR) analysis instead revealed that the sum of bacterial and fungal spores mass represented only a minor OMCOARSE fraction (<0.1%). X-ray photoelectron spectroscopic (XPS) analysis of C and N binding energies throughout the size fractions revealed an organic N increase in the PM10 compared to PM1 consistent with AMS observations.

Source Apportionment of Elemental Carbon in Beijing, China: Insights from Radiocarbon and Organic Marker Measurements.

Elemental carbon (EC) or black carbon (BC) in the atmosphere has a strong influence on both climate and human health. In this study, radiocarbon ((14)C) based source apportionment is used to distinguish between fossil fuel and biomass burning sources of EC isolated from aerosol filter samples collected in Beijing from June 2010 to May 2011. The (14)C results demonstrate that EC is consistently dominated by fossil-fuel combustion throughout the whole year with a mean contribution of 79% ± 6% (ranging from 70% to 91%), though EC has a higher mean and peak concentrations in the cold season. The seasonal molecular pattern of hopanes (i.e., a class of organic markers mainly emitted during the combustion of different fossil fuels) indicates that traffic-related emissions are the most important fossil source in the warm period and coal combustion emissions are significantly increased in the cold season. By combining (14)C based source apportionment results and picene (i.e., an organic marker for coal emissions) concentrations, relative contributions from coal (mainly from residential bituminous coal) and vehicle to EC in the cold period were estimated as 25 ± 4% and 50 ± 7%, respectively, whereas the coal combustion contribution was negligible or very small in the warm period.

Online determination of polycyclic aromatic hydrocarbon formation from a flame soot generator.

In this study, we produced a class of diffusion flame soot particles with varying chemical and physical properties by using the mini-Combustion Aerosol STandard (CAST) and applying varying oxidant gas flow rates under constant propane, quenching, and dilution gas supply. We varied the soot properties by using the following fuel-to-air equivalence ratios (Φ): 1.13, 1.09, 1.04, 1.00, 0.96, and 0.89. Within this Φ range, we observed drastic changes in the physical and chemical properties of the soot. Oxidant-rich flames (Φ < 1) were characterized by larger particle size, lower particle number concentration, higher black carbon (BC) concentration, lower brown carbon BrC.[BC](-1) than fuel-rich flames (Φ > 1). To investigate the polycyclic aromatic hydrocarbons (PAH) formation online, we developed a new method for quantification by using the one (13)C-containing doubly charged PAH ion in a high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS). The time-resolved concentration showed that the larger PAHs prevailed in the fuel-rich flames and diminished in the oxidant-rich flames. By comparison with the offline in situ derivatization-thermal-desorption gas-chromatography time-of-flight mass spectrometry (IDTD-GC-ToF-MS), we found that the concentration by using the HR-ToF-AMS was underestimated, especially for lower mass PAHs (C14-C18) in the fuel-rich flames possibly due to size limitation and degradation of semi-volatile species under high vacuum and desorption temperature in the latter. For oxidant-rich flames, the large PAHs (C20 and C22) were detected in the HR-ToF-AMS while it was not possible in IDTD-GC-ToF-MS due to matrix effect. The PAH formation was discussed based on the combination of our results and with respect to Φ settings.

Local incomplete combustion emissions define the PM2.5 oxidative potential in Northern India.

The oxidative potential (OP) of particulate matter (PM) is a major driver of PM-associated health effects. In India, the emission sources defining PM-OP, and their local/regional nature, are yet to be established. Here, to address this gap we determine the geographical origin, sources of PM, and its OP at five Indo-Gangetic Plain sites inside and outside Delhi. Our findings reveal that although uniformly high PM concentrations are recorded across the entire region, local emission sources and formation processes dominate PM pollution. Specifically, ammonium chloride, and organic aerosols (OA) from traffic exhaust, residential heating, and oxidation of unsaturated vapors from fossil fuels are the dominant PM sources inside Delhi. Ammonium sulfate and nitrate, and secondary OA from biomass burning vapors, are produced outside Delhi. Nevertheless, PM-OP is overwhelmingly driven by OA from incomplete combustion of biomass and fossil fuels, including traffic. These findings suggest that addressing local inefficient combustion processes can effectively mitigate PM health exposure in northern India.

Application of direct thermal desorption gas chromatography time-of-flight mass spectrometry for determination of nonpolar organics in low-volume samples from ambient particulate matter and personal samplers.

Direct thermal desorption and in-situ derivatization thermal desorption methods in conjunction with gas chromatography time-of-flight mass spectrometry have been characterized and evaluated for analysis of trace components from filters loaded with ambient particulate matter (PM). The limits of quantification were in the range of 7-24 pg for n-alkanes, 20 pg for hopanes, and 4-22 pg for polycyclic aromatic hydrocarbons (PAH). The limit of quantification was defined as the minimum amount of substance that conforms to the minimum distinguishable signal plus 9 times the standard deviation of this background signal from PM-loaded filters. The method has been successfully applied to low-volume samples from ambient PM collected with stationary and personal samplers. Stationary samples were collected in winter 2008 and 2010 in Augsburg, Germany. Sample aliquots of 0.2-0.3 m³ from stationary sampling were analyzed. High diurnal variation in concentration and source contribution was found especially during periods with low wind speed and low mixing layer height. High contributions of solid fuel combustion (wood and coal) were found in evening and nighttime samples, leading to peak PAH concentrations at midnight more than 10 times higher than at noon. Finally, the method was applied to samples collected by means of a personal sampler, i.e. a micro aethalometer, in Xi'an, China. Quantitative data on n-alkanes, hopanes, and PAH were obtained from sample volumes of 17 and 24 l. The impact of different sources such as vehicular and biogenic emissions could be distinguished.

Regional haze formation enhanced the atmospheric pollution levels in the Yangtze River Delta region, China: Implications for anthropogenic sources and secondary aerosol formation.

High-time-resolution (3-hour) PM2.5 samples were collected simultaneously from the rural and urban areas in the Yangtze River Delta region during winter. The aerosol samples were analyzed for carbonaceous components, organic tracers, water-soluble inorganic ions and stable carbon (δ13C) and nitrogen (δ15N) isotopic compositions of total carbon and total nitrogen. The values of PM2.5 and secondary organic carbon (SOC) for both sampling sites were observed 2 times higher in haze events compare to those in clear days, implying severe pollution occurred by photochemical oxidation during haze periods. The PM mass of rural samples showed similar temporal trend and significant correlation with the urban PM, reflecting pollution sources or their formation process are most likely identical. Diurnal variations of PM2.5 and carbonaceous components revealed that pollution levels increased at daytime due to the photochemical oxidation. In addition, SOC and OC were influenced by the relative humidity (RH%) and temperature (T °C), indicating that such meteorological factors play important roles in the occurrence of regional air pollution. The concentrations of levoglucosan, polycyclic aromatic hydrocarbons, hopanes, and n-alkanes were 625 ± 456 and 519 ± 301 ng m-3, 32.6 ± 24.7 and 28.7 ± 20.1 ng m-3, 1.83 ± 1.51 and 1.26 ± 1.34 ng m-3, and 302 ± 206 and 169 ± 131 ng m-3 for rural and urban samples, respectively. Levoglucosan is the most abundant organic compounds, exhibited 2-3 times higher in haze than clear days, suggesting biomass burning (BB) emission substantially affects the haze pollution in winter. Furthermore, NO3- was the dominant ionic species followed by SO42-, NH4+, Cl- and other minor species for both sites. The δ13C and δ15N values demonstrate that anthropogenic activities such as fossil fuel combustion and BB are the major sources for carbonaceous and nitrogenous aerosols. This study implies that both the regional anthropogenic emissions and meteorological conditions influenced the regional haze formation, leading enhancement of pollution levels in eastern China during winter.

Assessment of German population exposure levels to PM10 based on multiple spatial-temporal data.

Particulate matter is the key to increasing urban air pollution, and research into pollution exposure assessment is an important part of environmental health. In order to classify PM10 air pollution and to investigate the population exposure to the distribution of PM10, daily and monthly PM10 concentrations of 379 air pollution monitoring stations were obtained for a period from 01/01/2017 to 31/12/2017. Firstly, PM10 concentrations were classified using the head/tail break clustering algorithm to identify locations with elevated PM10 levels. Subsequently, population exposure levels were calculated using population-weighted PM10 concentrations. Finally, the power-law distribution was used to test the distribution of PM10 polluted areas. Our results indicate that the head/tail break algorithm, with an appropriate segmentation threshold, can effectively identify areas with high PM10 concentrations. The distribution of the population according to exposure level shows that the majority of people is living in polluted areas. The distribution of heavily PM10 polluted areas in Germany follows the power-law distribution well, but their boundaries differ from the boundaries of administrative cities; some even cross several administrative cities. These classification results can guide policymakers in dividing the country into several areas for pollution control.

Source apportionment of fine particulate matter in a Middle Eastern Metropolis, Tehran-Iran, using PMF with organic and inorganic markers.

With over 8 million inhabitants and 4 million motor vehicles on the streets, Tehran is one of the most crowded and polluted cities in the Middle East. Frequent exceedances of national daily PM2.5 limit have been reported in this city during the last decade, yet, the chemical composition and sources of fine particles are poorly determined. In the present study, 24-hour PM2.5 samples were collected at two urban sites during two separate campaigns, a one-year period from 2014 to 2015 and another three-month period at the beginning of 2017. Concentrations of organic carbon (OC), elemental carbon (EC), inorganic ions, trace metals and specific organic molecular markers were measured by chemical analysis of filter samples. The dominant mass components were organic matter (OM), sulfate and EC. With a 20% water-soluble organic carbon (WSOC) fraction, the predominance of primary anthropogenic sources (i.e. fossil fuel combustion) was anticipated. A positive matrix factorization (PMF) analysis using the ME-2 (Multilinear Engine-2) solver was then applied to this dataset. 5 factors were identified by Marker-PMF, named as traffic exhaust (TE), biomass burning (BB), industries (Ind.), nitrate-rich and sulfate-rich. Another 4 factors were identified by Metal-PMF, including, dust, vehicles (traffic non-exhaust, TNE), industries (Ind.) and heavy fuel combustion (HFC). Traffic exhaust was the dominant source with 44.5% contribution to total quantified PM2.5 mass. Sulfate-rich (24.2%) and nitrate-rich (18.4%) factors were the next major contributing sources. Dust (4.4%) and biomass burning (6.7%) also had small contributions while the total share of all other factors was < 2%. Investigating the correlations of different factors between the two sampling sites showed that traffic emissions and biomass burning were local, whereas dust, heavy fuel combustion and industrial sources were regional. Results of this study indicate that gas- and particle-phase pollutants emitted from fossil fuel combustion (mobile and stationary) are the principal origin of both primary and secondary fine aerosols in Tehran.

Impact of photochemical ageing on Polycyclic Aromatic Hydrocarbons (PAH) and oxygenated PAH (Oxy-PAH/OH-PAH) in logwood stove emissions.

The combustion of spruce logwood in a modern residential stove was found to emit polycyclic aromatic hydrocarbons (PAH) and oxygenated polycyclic aromatic hydrocarbons (OPAH) with emission factors of 404 µg MJ-1 of 35 analysed PAH, 317 µg MJ-1 of 11 analysed Oxy-PAH and 12.5 µg MJ-1 of 5 analysed OH-PAH, most of which are known as potential mutagens and carcinogens. Photochemical ageing in an oxidation flow reactor (OFR) degraded particle-bound PAH, which was also reflected in declining PAH toxicity equivalent (PAH-TEQ) values by 45 to 80% per equivalent day of photochemical ageing in the atmosphere. OPAH concentrations decreased less than PAH concentrations during photochemical ageing, supposedly due to their secondary formation, while 1-hydroxynaphthalene, 1,5-dihydroxynaphthalene and 1,8-naphthalaldehydic acid were significantly increased after ageing. Furthermore, secondary organic aerosol (SOA) formation and aromatic compounds not included in targeted analysis were investigated by thermal-optical carbon analysis (TOCA) hyphenate to resonance-enhanced multi-photon ionisation time-of-flight mass spectrometry (REMPI-TOFMS). The commonly used PAH-source indicators phenanthrene/anthracene, fluoranthene/pyrene, retene/chrysene, and indeno[cd]pyrene/benzo[ghi]perylene remained stable during photochemical ageing, enabling identification of wood combustion emissions in ambient air. On the other hand, benz[a]pyrene/benz[e]pyrene and benz[a]anthracene/chrysene were found to decrease with increasing photochemical age. Retene/chrysene was not a proper classifier for the wood combustion emissions of this study, possibly due to more efficient combustion than in open wood burning, from which this diagnostic ratio was initially derived. This study motivates in-depth investigation of degradation kinetics of particle-bound species on different combustion aerosol as well as the consequences of photochemical ageing on toxicity and identification of wood combustion emissions in ambient air.

PM2.5 concentration and composition in the urban air of Nanjing, China: Effects of emission control measures applied during the 2014 Youth Olympic Games.

Industrial processes, coal combustion, biomass burning (BB), and vehicular transport are important sources of atmospheric fine particles (PM2.5) and contribute to ambient air concentrations of health-hazardous species, such as heavy metals, polycyclic aromatic hydrocarbons (PAH), and oxygenated-PAHs (OPAH). In China, emission controls have been implemented to improve air quality during large events, like the Youth Olympic Games (YOG) in August 2014 in Nanjing. In this work, six measurement campaigns between January 2014 and August 2015 were undertaken in Nanjing to determine the effects of emission controls and meteorological factors on PM2.5 concentration and composition. PAHs, OPAHs, hopanes, n­alkanes, heavy metals, and several other inorganic elements were measured. PM2.5 and potassium concentrations were the highest in May-June 2014 indicating the prevalence of BB plumes in Nanjing. Emission controls substantially reduced concentrations of PM2.5 (31%), total PAHs (59%), OPAHs (37%), and most heavy metals (44-89%) during the YOG compared to August 2015. In addition, regional atmospheric transport and meteorological parameters partly explained the observed differences between the campaigns. The most abundant PAHs and OPAHs were benzo[b,k]fluoranthenes, fluoranthene, pyrene, chrysene, 1,8­naphthalic anhydride, and 9,10­anthracenedione in all campaigns. Carbon preference index and the contribution of wax n­alkanes indicated mainly biogenic sources of n­alkanes in May-June 2014 and anthropogenic sources in the other campaigns. Hopane indexes pointed to vehicular transport as the major source of hopanes, but contribution of coal combustion was detected in winter 2015. The results provide evidence to the local government of the impacts of the air protection regulations. However, differences between individual components were observed, e.g., concentrations of potentially more harmful OPAHs decreased less than concentrations of PAHs. The results suggest that the proportions of hazardous components in the PM2.5 may also change considerably due to emission control measures.

Organic speciation of ambient quasi-ultrafine particulate matter (PM0.36) in Augsburg, Germany: Seasonal variability and source apportionment.

To investigate the organic composition and their sources of very fine atmospheric particulate matter (PM), size-segregated PM was sampled using rotating drum impactor (RDI) in series with a sequential filter sampler in Augsburg, Germany, from April 2014 to February 2015. Organic speciation analysis and organic carbon/elemental carbon (OC/EC) analysis was performed for the smallest size fraction PM0.36 (PM<360nm). Different OC fractions were determined by thermal optical EC/OC analyzer, and OC2, OC3 and OC4 refer to OC fractions that were derived at 280, 480 and 580°C, respectively. Positive matrix factorization (PMF) analysis was applied for source apportionment study. PMF resolved 5 sources including biogenic dominated secondary organic aerosol (bioSOA), isoprene dominated SOA (isoSOA), traffic, biomass burning (BB) and biomass burning originated SOA (bbSOA). On annual average, PMF results indicate the largest contribution of biogenic originated SOA (bioSOA plus isoSOA) to OC, followed by traffic and then BB related sources (BB plus bbSOA). Traffic was found to be associated with the smallest particles; whereas bioSOA and BB are associated with larger particles. Secondary organic marker compounds from biogenic precursors, OC2, OC3 and bioSOA, isoSOA source factors show summer maximum. Polycyclic aromatic hydrocarbons (PAHs), biomass burning markers, OC4 and BB, bbSOA source factors show winter maximum. Hopanes and the traffic source factor show little seasonal variation. Summer peaks of OC3 and OC2 are well modeled by PMF and are attributed mainly to biogenic SOA. OC4 was generally poorly modeled due to lack of characteristic low volatile markers. Summer maxima of biogenic SOA related compounds and source factors are positively correlated with temperature, global radiation, O3 concentration and mixing layer height (MLH). Winter maxima of BB related compounds and source factors are negatively correlated with temperature and MLH; whereas positively correlated with NO2 level.

Chemical composition and speciation of particulate organic matter from modern residential small-scale wood combustion appliances.

Combustion technologies of small-scale wood combustion appliances are continuously developed decrease emissions of various pollutants and increase energy conversion. One strategy to reduce emissions is the implementation of air staging technology in secondary air supply, which became an established technique for modern wood combustion appliances. On that account, emissions from a modern masonry heater fuelled with three types of common logwood (beech, birch and spruce) and a modern pellet boiler fuelled with commercial softwood pellets were investigated, which refer to representative combustion appliances in northern Europe In particular, emphasis was put on the organic constituents of PM2.5, including polycyclic aromatic hydrocarbons (PAHs), oxygenated PAHs (OPAHs) and phenolic species, by targeted and non-targeted mass spectrometric analysis techniques. Compared to conventional wood stoves and pellet boilers, organic emissions from the modern appliances were reduced by at least one order of magnitude, but to a different extent for single species. Hence, characteristic ratios of emission constituents and emission profiles for wood combustion identification and speciation do not hold for this type of advanced combustion technology. Additionally, an overall substantial reduction of typical wood combustion markers, such as phenolic species and anhydrous sugars, were observed. Finally, it was found that slow ignition of log woods changes the distribution of characteristic resin acids and phytosterols as well as their thermal alteration products, which are used as markers for specific wood types. Our results should be considered for wood combustion identification in positive matrix factorisation or chemical mass balance in northern Europe.

Spatial and temporal variation of sources contributing to quasi-ultrafine particulate matter PM0.36 in Augsburg, Germany.

OBJECTIVE: to study the sources contributing to quasi-ultrafine particle (UFP) organic carbon and the spatial temporal variability of the sources. METHOD: 24h quasi-UFP (particulate matter <0.36µm in this study) was sampled at a reference site continuously and at one of 5 other sites (T1, T2, T3, T4 and B1) in parallel in Augsburg, Germany from April 11th, 2014 to February 22nd, 2015, attempting to conduct 2-week campaigns at each site in 3 different seasons. Positive matrix factorization (PMF) was applied to measured organic tracers for source apportionment analyses. Pearson correlation coefficient r and coefficient of divergence (COD) were calculated to investigate spatial temporal variation of source contributions. RESULT: 5 sources were identified comprising biomass burning (BB), traffic emissions (Traffic), biogenic secondary organic aerosol (bioSOA), isoprene originated secondary organic aerosol (isoSOA) and biomass burning related secondary organic aerosol (bbSOA). In general, good temporal correlation and uniform distribution within the study area are found for bioSOA and bbSOA, probably resulting from regional formation/transport. Lower temporal correlation and spatial heterogeneity of isoSOA were found at the city background site with local influence from green space and less traffic impact. BB demonstrated very good temporal correlation, but higher contributions at sites influenced by local residential heating emissions were observed. Traffic showed the least seasonality and lower correlation over time among the sources. However, it demonstrated low spatial heterogeneity of absolute contribution, and only a few days of elevated contribution was found at T3 when wind came directly from the street nearby. CONCLUSION: temporal correlation and spatial variability of sources contributing to the organic fraction of quasi-UFP vary among sites and source types and show source-specific characteristics. Therefore, caution should be taken when using one monitor site measurement to assess human exposure in health effect studies of quasi-UFP.