Sources and characteristics of carbonaceous aerosol in two largest cities in Pearl River Delta Region,China

PM_2.5 samples were collected at five sites in Guangzhou and Hong Kong, Pearl River Delta Region (PRDR), China in both summer and winter during 2004–2005. Elemental carbon (EC) and organic carbon (OC) in these samples were measured. The OC and EC concentrations ranked in the order of urban Guangzhou > urban Hong Kong > background Hong Kong. Total carbonaceous aerosol (TCA) contributed less to PM_2.5 in urban Guangzhou (32–35%) than that in urban Hong Kong (43–57%). The reason may be that, as an major industrial city in South China, Guangzhou would receive large amount of inorganic aerosol from all kinds of industries, however, as a trade center and seaport, urban Hong Kong would mainly receive organic aerosol and EC from container vessels and heavy-duty diesel trucks. At Hong Kong background site Hok Tsui, relatively lower contribution of TCA to PM_2.5 may result from contributions of marine inorganic aerosol and inland China pollutant. Strong correlation (R²=0.76–0.83) between OC and EC indicates minor fluctuation of emission and the secondary organic aerosol (SOA) formation in urban Guangzhou. Weak correlation between OC and EC in Hong Kong can be related to the impact of the long-range transported aerosol from inland China. Averagely, secondary OC (SOC) concentrations were 3.8–5.9 and 10.2–12.8 μg m⁻³, respectively, accounting for 21–32% and 36–42% of OC in summer and winter in Guangzhou. The average values of 4.2–6.8% for SOA/ PM_2.5 indicate that SOA was minor component in PM_2.5 in Guangzhou.     

Chemical characteristics of principal PM2.5 species in Chongju,South Korea

Fine particles were collected over four seasons from October 1995 to August 1996 to evaluate the chemical characteristics of principal PM_2.5 components in Chongju, South Korea. The annual mean concentrations of PM_2.5 (d_p⩽2.5 μm), sulfate, nitrate, ammonium, elemental carbon (EC) and organic carbon (OC) were 44.2, 8.22, 3.63, 2.84, 4.44 and 4.99 μg m⁻³, respectively. The sum of the species measured from this study accounted for 50–62% of the PM_2.5 mass. Sulfate was the most abundant species and constituted 13–23% of the PM_2.5 mass. The EC and OC accounted for 17–28% of PM_2.5. The correlation between OC and EC was strong, and the annual mean ratio of OC/EC was 1.12, suggesting that OC measured in the Chongju area may be emitted directly in particulate form as a primary aerosol.     

Multi-year hourly PM2.5 carbon measurements in New York: Diurnal,day of week and seasonal patterns

Multi-year hourly measurements of PM_2.5 elemental carbon (EC) and organic carbon (OC) from a site in the South Bronx, New York were used to examine diurnal, day of week and seasonal patterns. The hourly carbon measurements also provided temporally resolved information on sporadic EC spikes observed predominantly in winter. Furthermore, hourly EC and OC data were used to provide information on secondary organic aerosol formation. Average monthly EC concentrations ranged from 0.5 to 1.4 μg m^?3 with peak hourly values of several μg m^?3 typically observed from November to March. Mean EC concentrations were lower on weekends (approximately 27% lower on Saturday and 38% lower on Sunday) than on weekdays (Monday to Friday). The weekday/weekend difference was more pronounced during summer months and less noticeable during winter. Throughout the year EC exhibited a similar diurnal pattern to NO_x showing a pronounced peak during the morning commute period (7–10 AM EST). These patterns suggest that EC was impacted by local mobile emissions and in addition by emissions from space heating sources during winter months. Although EC was highly correlated with black carbon (BC) there was a pronounced seasonal BC/EC gradient with summer BC concentrations approximately a factor of 2 higher than EC. Average monthly OC concentrations ranged from 1.0 to 4.1 μg m^?3 with maximum hourly concentrations of 7–11 μg m^?3 predominantly in summer or winter months. OC concentrations generally correlated with PM_2.5 total mass and aerosol sulfate and with NO_x during winter months. OC showed no particular day of week pattern. The OC diurnal pattern was typically different than EC except in winter when OC tracked EC and NO_x indicating local primary emissions contributed significantly to OC during winter at the urban location. On average secondary organic aerosol was estimated to account for 40–50% of OC during winter and up to 63–73% during summer months.     

Characteristics of vertical profiles and sources of PM2.5, PM10 and carbonaceous species in Beijing

In August 2003 during the anticipated month of the 2008 Beijing Summer Olympic Games, we simultaneously collected PM₁₀ and PM_2.5 samples at 8, 100, 200 and 325 m heights up a meteorological tower and in an urban and a suburban site in Beijing. The samples were analysed for organic carbon (OC) and elemental carbon (EC) contents. Particulate matter (PM) and carbonaceous species pollution in the Beijing region were serious and widespread with 86% of PM_2.5 samples exceeding the daily National Ambient Air Quality Standard of the USA (65 μg m⁻³) and the overall daily average PM₁₀ concentrations of the three surface sites exceeding the Class II National Air Quality Standard of China (150 μg m⁻³). The maximum daily PM_2.5 and PM₁₀ concentrations reached 178.7 and 368.1 μg m⁻³, respectively, while those of OC and EC reached 22.2 and 9.1 μg m⁻³ in PM_2.5 and 30.0 and 13.0 μg m⁻³ in PM₁₀, respectively. PM, especially PM_2.5, OC and EC showed complex vertical distributions and distinct layered structures up the meteorological tower with elevated levels extending to the 100, 200 and 300 m heights. Meteorological evidence suggested that there exist fine atmospheric layers over urban Beijing. These layers were featured by strong temperature inversions close to the surface (<50 m) and more stable conditions aloft. They enhanced the accumulation of pollutants and probably caused the complex vertical distributions of PM and carbonaceous species over urban Beijing. The built-up of PM was accompanied by transport of industrial emissions from the southwest direction of the city. Emissions from road traffic and construction activities as well as secondary organic carbon (SOC) are important sources of PM. High OC/EC ratios (range of 1.8–5.1 for PM_2.5 and 2.0–4.3 for PM₁₀) were found, especially in the higher levels of the meteorological tower suggesting there were substantial productions of SOC in summer Beijing. SOC is estimated to account for at least 33.8% and 28.1% of OC in PM_2.5 and PM₁₀, respectively, with higher percentages at the higher levels of the tower.     

Carbon content of atmospheric aerosols in a residential area during the wood combustion season in Sweden

Carbonaceous aerosol particles were observed in a residential area with wood combustion during wintertime in Northern Sweden. Filter samples were analyzed for elemental carbon (EC) and organic carbon (OC) content by using a thermo-optical transmittance method. The light-absorbing carbon (LAC) content was determined by employing a commercial Aethalometer and a custom-built particle soot absorption photometer. Filter samples were used to convert the optical signals to LAC mass concentrations. Additional total PM₁₀ mass concentrations and meteorological parameters were measured. The mean and standard deviation mass concentrations were 4.4±3.6 μg m⁻³ for OC, and 1.4±1.2 μg m⁻³ for EC. On average, EC accounted for 10.7% of the total PM₁₀ and the contribution of OC to the total PM₁₀ was 35.4%. Aethalometer and custom-built PSAP measurements were highly correlated (R²=0.92). The hourly mean value of LAC mass concentration was 1.76 μg m⁻³ (median 0.88 μg m⁻³) for the winter 2005–2006. This study shows that the custom-built PSAP is a reliable alternative for the commercial Aethalometer with the advantage of being a low-cost instrument.     

Characterisation of PM10 atmospheric aerosols for the wet season 2005 at two sites in East Africa

Ambient daily PM₁₀ aerosol samples were collected at two sites in Tanzania in May and June 2005 (during the wet season), and their chemical characteristics were studied. The sites were a rural site in Morogoro and an urban kerbside site in Dar es Salaam. A Gent PM₁₀ stacked filter unit sampler with sequential Nuclepore polycarbonate filters, providing fine and coarse size fractions, and a PM₁₀ sampler with quartz fibre filters were deployed. Parallel collections of 24 h were made with the two samplers and the number of these collections was 13 in Morogoro and 16 in Dar es Salaam. The average mass concentration of PM₁₀ was 27 ± 11 μg/m³ in Morogoro and 51 ± 21 μg/m³ in Dar es Salaam. In Morogoro, the mean concentrations of organic carbon (OC), elemental carbon (EC), and water-soluble organic carbon (WSOC) were 6.8, 0.51, and 2.8 μg/m³, respectively. In contrast, higher mean concentrations (11.9, 4.6, and 3.3 μg/m³, respectively) were obtained for Dar es Salaam. At both sites, species and elements, such as black carbon, NH₄⁺, non-sea-salt SO₄^2?, K, and Ni (and at Dar es Salaam also V, As, Br, and Pb) were mainly present in the fine size fraction. The common crustal and sea-salt elements, including Na, Mg, Al, Si, Cl, Ca, Ti, Mn, Fe, and Sr, and also NO₃^? and P (and to a lesser extent Cu and Zn) were concentrated in the coarse particles. Aerosol chemical mass closure indicated that the PM₁₀ mass in Morogoro consisted, on average, of 48% organic matter (OM), 44% crustal matter, 4% sea salt, and 2% EC, while in Dar es Salaam OM, crustal matter, sea salt, and EC represented 37%, 32%, 9%, and 9% of the PM₁₀ mass. The contributions of the secondary inorganic aerosol (non-sea-salt sulphate, nitrate, and ammonium) were small, i.e., only 5% in total at each site. Carbonaceous materials and crustal matter were thus the most important components of the PM₁₀ mass. It is suggested that biomass burning is a major contributor to the OM; at Dar es Salaam there is also a very substantial contribution from traffic. A source apportionment calculation indicated that 68% of the OC at this site originated from traffic exhaust versus 32% from charcoal burning. The crustal matter at Morogoro is likely mainly attributable to soil dust resuspension, whereas in Dar es Salaam it is likely mostly resuspended road dust.     

Carbonaceous and inorganic composition in long-range transported aerosols over northern Japan: Implication for aging of water-soluble organic fraction

To better understand the influence of sources and atmospheric processing on aerosol chemical composition, we collected atmospheric particles in Sapporo, northern Japan during spring and early summer 2005 under the air mass transport conditions from Siberia, China and surrounding seas. The aerosols were analyzed for inorganic ions, organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and the major water-soluble organic compound classes (i.e., dicarboxylic acids and sugars). SO₄^2? is the most abundant inorganic constituent (average 44% of the identified inorganic ion mass) followed by NH₄⁺ (21%) and NO₃^? (13%). Concentrations of OC, EC, and WSOC ranged from 2.0–16, 0.24–2.9, and 0.80–7.9 μg m^?3 with a mean of 7.4, 1.0, and 3.1 μg m^?3, respectively. High OC/EC ratios (range: 3.6–19, mean: 8.7) were obtained, however WSOC/OC ratios (0.23–0.69, 0.44) do not show any significant diurnal changes. These results suggest that the Sapporo aerosols were already aged, but were not seriously affected by local photochemical processes. Identified water-soluble organic compounds (diacids + sugars) account for <10% of WSOC. Based on some marker species and air mass back trajectory analyses, and using stable carbon isotopic compositions of shorter-chain diacids (i.e., C₂–C₄) as photochemical aging factor of organic aerosols, the present study suggests that a fraction of WSOC in OC is most likely influenced by aerosol aging, although the OC loading in aerosols may be more influenced by their sources and source regions.     

Comparative analysis of organic and elemental carbon concentrations in carbonaceous aerosols in three European cities

Sampling and analysis of carbonaceous compounds in particulate matter presents a number of difficulties related to artefacts during sampling and to the distinction between organic (OC) and elemental carbon (EC) during analysis. Our study reports on a comparative analysis of OC, EC and WSOC (water-soluble organic carbon) concentrations, as well as sampling artefacts, for PM2.5 aerosol in three European cities (Amsterdam, Barcelona and Ghent) representing Southern and Western European urban environments. Comparability of results was ensured by using a single system for sample analysis from the different sites. OC and EC concentrations were higher in the vicinity of roads, thus having higher levels in Amsterdam (3.9–6.7 and 1.7–1.9 μg m⁻³, respectively) and Barcelona (3.6–6.9 and 1.5–2.6 μg m⁻³) than in Ghent (2.7–5.4 and 0.8–1.2 μg m⁻³). A relatively larger influence of secondary organic aerosols (SOA), as deduced from a larger OC/EC ratio, was observed in Ghent. In absolute sense, WSOC concentrations were similar at the three sites (1.0–2.3 μg m⁻³). Positive artefacts were higher in Southern (11–16% of the OC concentration in Barcelona) than in Western Europe (5–12% in Amsterdam, 5–7% in Ghent). During special episodes, the contribution of carbonaceous aerosols from non-local sources accounted for 67–69% of the OC concentration in Western Europe, and for 44% in Southern Europe.     

Investigation of the motor vehicle exhaust contribution to primary fine particle organic carbon in urban air

Motor vehicle (MV) emissions and ambient particle concentrations under a variety of situations were studied in Toronto and Vancouver, Canada. Petroleum biomarkers (i.e., hopanes and steranes) were used to determine the fraction of fine particle organic carbon (OC) attributed to primary particles in MV exhaust. Source profiles obtained from a tunnel and from direct tailpipe emissions were applied to ambient measurements at locations ranging from rush hour traffic to a regional background site. The greatest amount of MV OC, 4.0 μgC m⁻³ out of 9.1 μgC m⁻³ or 43%, was observed 75 m south of a commuter highway during a period that included morning rush hour. Monthly estimates of MV-OC were determined for a downtown Toronto monitoring site for 2 years. Total OC concentrations were greater in the summer, due to secondary OC, but the amount of MV-OC did not exhibit a strong seasonal pattern. However, on a per cent basis, MV contributions from primary OC emissions were greatest in the winter (15–20%) and smallest in the summer (10–15%) with a two-year average of 14% of the OC or about 5% of the PM_2.5.     

Characterisation of fresh particulate vehicular exhausts near a Paris high flow road

Simultaneous continuous measurements of PM_2.5, PM₁₀, black carbon mass (BCae), Black smoke (BS) and particle number density (N) were conducted in the close vicinity of a high traffic road around Paris during a three-month period beginning in August 1997. In parallel some aerosol collection was performed on filters in order to assess the black carbon (BC), organic carbon (OC) and water soluble organic fractions (WSOC) of the freshly emitted traffic aerosols. The high hourly concentrations of PM_2.5 (39±20 μg m⁻³), BCae (14±7 μg m⁻³), and N (220,000±115,000 cm⁻³), were found to be well correlated with each other. On average PM_2.5 represented 66±13% of PM₁₀ and appears to be composed primarily of BC (43±20%). On the contrary no correlation was found between PM_2.5 and the coarse (PM₁₀–PM_2.5) mass fractions which was attributed to resuspension processes by vehicles. Black carbon mass concentrations obtained from both filter analyses (BC) and Aethalometre data (BCae) show a good agreement suggesting that the Aethalometre calibration based on a black carbon specific attenuation coefficient (σ) of 19 m² g⁻¹ is well adapted to nearby roadside measurements. Daily BC (used as a surrogate for fine particles) concentrations and wind speed were found to be anti-correlated. Average daily variations of BC could be related to traffic intensity and regime as well as to the boundary layer height. As expected for freshly emitted traffic aerosols, filter analyses indicated a high BC/TC ratio (29±5%) and a low mean WSOC/OC ratio (12.5±5%) for the bulk aerosol. For these two ratios no day/night differences were observed, the sampling station being probably too close to traffic to evidence photochemical modification of the aerosol phase. Finally, a linear relationship was found between BC and BS hourly concentrations (BC=0.10×BS+1.18; r²=0.93) which offers interesting perspectives to retrieve BC concentrations from existing BS archives.     

Polychlorinated biphenyls and particulate organic/elemental carbon in the atmosphere of Chesapeake Bay,USA

Polychlorinated biphenyls (PCBs) and particulate organic/elemental carbon (OC/EC) differ as to sources, but are both elevated in major urban areas leading to loadings of proximate terrestrial and aquatic systems. Because of the dramatic difference in speciation, sources, and sinks of these compunds, gas+particulate phase PCBs and particulate OC/EC were measured in urban Baltimore, MD and over Chesapeake Bay at 4 and 12 h frequencies in July 1997. Gas phase ∑PCBs averaged 1180 pg m⁻³ for Baltimore and 550 pg m⁻³ for northern Chesapeake Bay. PCB homolog distributions in the gas phase differed between the land and over-water sites whereby the trichlorobiphenyls were higher in Baltimore compared to Chesapeake Bay. Autocorrelation analysis yielded a diurnal cycle for gas phase PCBs at Baltimore with the lowest concentrations observed during the day. Particulate organic and elemental carbon constituted 12.4% (17.4% organic matter) and 2.8% of total suspended particles (TSP) in Baltimore, and 15.0% (21.0% organic matter) and 5.3% over the Chesapeake Bay, respectively. Variability in PCB concentrations was not related to the variability in OC/EC concentrations. OC/EC ratios suggest that particulate organic carbon was mostly primary aerosol. Emissions of both classes of compounds into the Baltimore atmosphere and vicinity are major sources to the Bay.     

Fine particle concentrations and composition during wintertime inversions in Logan,Utah, USA

During Winter 2004, a series of elevated PM_2.5 events occurred in Logan, Utah, coinciding with strong winter inversions. This period resulted in 17 exceedances of the 24-h PM_2.5 standard, and some of the highest PM_2.5 mass loadings recorded in the United States, including 9 days of 24-h PM_2.5 measurements over 100 μg m⁻³. During the 3-month period, we monitored the size and mass concentrations of airborne particles using an aerosol mass spectrometer. PM_2.5 concentrations were dominated by the formation of ammonium nitrate, accounting for over 50% of the non-refractory aerosol matter throughout the study and 80% on the highest pollution days. Another 15–20% of the particulate matter was composed of organic carbon. The high particle concentration loadings in Utah's Cache Valley result from a combination of unfavorable meteorology dominated by a severe cold-temperature inversion, a mix of rural and urban emission sources, and a confined geographical area. As a rapidly growing formerly rural area, the Cache Valley is representative of future air pollution problems facing areas of the interior west undergoing rapid urbanization.     

Characterization of PM2.5-bound polycyclic aromatic hydrocarbons in Atlanta

Twenty-four hour PM_2.5 samples from a rural site, an urban site, and a suburban site (next to a major highway) in the metropolitan Atlanta area in December 2003 and June 2004 were analyzed for 19 polycyclic aromatic hydrocarbons (PAH). Extraction of the air samples was conducted using an accelerated solvent extraction method followed by isotope dilution gas chromatography/mass spectrometry determination. Distinct seasonal variations were observed in total PAH concentration (i.e. significantly higher concentrations in December than in June). Mean concentrations for total particulate PAHs in December were 3.16, 4.13, and 3.40 ng m^?3 for the urban, suburban and rural sites, respectively, compared with 0.60, 0.74, and 0.24 ng m^?3 in June. Overall, the suburban site, which is impacted by a nearby major highway, had higher PAH concentration than did the urban site. Total PAH concentrations were found to be well correlated with PM_2.5, organic carbon (OC), and elemental carbon (EC) in both months (r² = 0.36–0.78, p < 0.05), although the slopes from the two months were different. PAHs represented on average 0.006% of total PM_2.5 mass and 0.017% of OC in June, compared with 0.033% of total PM_2.5 and 0.14% of OC in December. Total PAH concentrations were also correlated with potassium ion (r² = 0.39, p = 0.014) in December, but not in June, suggesting that in winter biomass burning can potentially be an important source for particulate PAH. Retene was found at a higher median air concentration at the rural site than at the urban and suburban sites—unlike the rest of the PAHs, which were found at lower levels at the rural site. Retene also had a larger seasonal difference and had the weakest correlation with the rest of the PAHs measured, suggesting that retene, in particular, might be associated with biomass burning.     

Characteristics of PM2.5 carbonaceous aerosol in the Sihwa industrial area,Korea

In order to investigate the characteristics of carbonaceous fine aerosols, PM_2.5 particulate samples were collected in the Sihwa industrial complex area between February 1998 and 1999 and in Seoul between 31 May and 9 June 1999, respectively. The carbonaceous species were analyzed by the selective thermal manganese dioxide oxidation (TMO) method. In Sihwa, average OC and EC concentrations for the entire data set were measured to be 9.8 and 1.8 μg m⁻³, respectively. The OC concentrations were higher than those measured in other urban environments. The EC concentrations were lower than those of other urban environments. The OC/EC ratio measured at the Sihwa area was higher than those at other urban and rural environments. Backward trajectories of sampled air masses were performed to find out the sources of those higher OC/EC levels. Enrichment in the organic compounds during winter periods can be explained by the combination of primary local emissions from the industrial complex area and long-range transport of organic species from outside the Sihwa area. High OC values in June resulted from primary anthropogenic emissions and secondary organic aerosol formation rather than the atmospheric transport of organic compounds from the outside. In urban area of Seoul, the OC and EC concentrations in PM_2.5 during the summer were higher than those measured at other urban atmospheres. OC/EC ratios obtained in Seoul were lower than Sihwa. It can be concluded that carbonaceous species in Seoul were mainly emitted from primary anthropogenic sources.     

Chemical characterization and source apportionment of fine and coarse particulate matter in Lahore,Pakistan

Lahore, Pakistan is an emerging megacity that is heavily polluted with high levels of particle air pollution. In this study, respirable particulate matter (PM_2.5 and PM₁₀) were collected every sixth day in Lahore from 12 January 2007 to 19 January 2008. Ambient aerosol was characterized using well-established chemical methods for mass, organic carbon (OC), elemental carbon (EC), ionic species (sulfate, nitrate, chloride, ammonium, sodium, calcium, and potassium), and organic species. The annual average concentration (±one standard deviation) of PM_2.5 was 194 ± 94 μg m^?3 and PM₁₀ was 336 ± 135 μg m^?3. Coarse aerosol (PM_10?2.5) was dominated by crustal sources like dust (74 ± 16%, annual average ± one standard deviation), whereas fine particles were dominated by carbonaceous aerosol (organic matter and elemental carbon, 61 ± 17%). Organic tracer species were used to identify sources of PM_2.5 OC and chemical mass balance (CMB) modeling was used to estimate relative source contributions. On an annual basis, non-catalyzed motor vehicles accounted for more than half of primary OC (53 ± 19%). Lesser sources included biomass burning (10 ± 5%) and the combined source of diesel engines and residual fuel oil combustion (6 ± 2%). Secondary organic aerosol (SOA) was an important contributor to ambient OC, particularly during the winter when secondary processing of aerosol species during fog episodes was expected. Coal combustion alone contributed a small percentage of organic aerosol (1.9 ± 0.3%), but showed strong linear correlation with unidentified sources of OC that contributed more significantly (27 ± 16%). Brick kilns, where coal and other low quality fuels are burned together, are suggested as the most probable origins of unapportioned OC. The chemical profiling of emissions from brick kilns and other sources unique to Lahore would contribute to a better understanding of OC sources in this megacity.     

Emission factors of PAHs,methoxyphenols, levoglucosan,elemental carbon and organic carbon from simulated wheat and Kentucky bluegrass stubble burns

Emission factors (EFs) of pollutants from post-harvest agricultural burning are required for predicting downwind impacts of smoke and inventorying emissions. EFs of polycyclic aromatic hydrocarbons (PAH), methoxyphenols (MP), levoglucosan (LG), elemental carbon (EC) and organic carbon (OC) from wheat and Kentucky bluegrass (KBG) stubble burning were quantified in a US EPA test burn facility. The PAH and MP EFs for combined solid+gas phases are 17±8.2 mg kg⁻¹ and 79±36 mg kg⁻¹, respectively, for wheat and 21±15 mg kg⁻¹ and 35±24 mg kg⁻¹, respectively, for KBG. LG, particulate EC and artifact-corrected OC EFs are 150±130 mg kg⁻¹, 0.35±0.16 g kg⁻¹ and 1.9±1.1 g kg⁻¹, respectively, for wheat and 350±510 mg kg⁻¹, 0.63±0.056 g kg⁻¹ and 6.9±0.85 g kg⁻¹, respectively, for KBG. Positive artifacts associated with OC sampling were evaluated and remedied with a two-filter system. EC and OC accounted for almost two-thirds of PM_2.5 mass, while LG accounted for just under 3% of the PM_2.5 mass. Since EFs of these pollutants generally decreased with increasing combustion efficiency (CE), identifying and implementing methods of increasing the CEs of burns would help reduce their emissions from agricultural field burning. PAH, OC and EC EFs are comparable to other similar studies reported in literature. MP EFs appear dependent on the stubble type and are lower than the EFs for hard and softwoods reported in literature, possibly due to the lower lignin content in wheat and KBG.     

Chemical composition of aerosols during a major biomass burning episode over northern Europe in spring 2006: Experimental and modelling assessments

The long-range transported smokes emitted by biomass burning had a strong impact on the PM_2.5 mass concentrations in Helsinki over the 12 days period in April and May 2006. To characterize aerosols during this period, the real-time measurements were done for PM_2.5, PM_2.5–10, common ions and black carbon. Moreover, the 24-h PM₁ filter samples were analysed for organic and elemental carbon (OC and EC), water-soluble organic carbon (WSOC), ions and levoglucosan. The Finnish emergency and air quality modelling system SILAM was used for the forecast of the PM_2.5 concentration generated by biomass burning. According to the real-time PM_2.5 data, the investigated period was divided into four types of PM situations: episode 1 (EPI-1; 25–29 April), episode 2 (EPI-2; 1–5 May), episode 3 (EPI-3; 5–6 May) and a reference period (REF; 24 March–24 April). EPI-3 included a local warehouse fire and therefore it is discussed separately. The PM₁ mass concentrations of biomass burning tracers—levoglucosan, potassium and oxalate—increased during the two long-range transport episodes (EPI-1 and EPI-2). The most substantial difference between the episodes was exhibited by the sulphate concentration, which was 4.9 (±1.4) μg m⁻³ in EPI-2 but only 2.4 (±0.31) μg m⁻³ in EPI-1 being close to that of REF (1.8±0.54 μg m⁻³). The concentration of particulate organic matter in PM₁ was clearly higher during EPI-1 (11±3.3 μg m⁻³) and EPI-2 (9.7±4.0 μg m⁻³) than REF (1.3±0.45 μg m⁻³). The long-range transported smoke had only a minor impact on the WSOC-to-OC ratio. According to the model simulations, MODIS detected the fires that caused the first set of concentration peaks (EPI-1) and the local warehouse fire (EPI-3), but missed the second one (EPI-2) probably due to dense frontal clouds.     

A wintertime PM2.5 episode at the Fresno,CA, supersite

A winter PM_2.5 episode that achieved a maximum 24-h average of 138 μg m⁻³ at the Fresno Supersite in California's San Joaquin Valley between 2 and 12 January, 2000 is examined using 5-min to 1-h continuous measurements of mass, nitrate, black carbon, particle-bound PAH, and meteorological measurements. Every day PM_2.5 sampling showed that many episodes, including this one, are missed by commonly applied sixth-day monitoring, even though quarterly averages and numbers of US air quality standard exceedances are adequately estimated. Simultaneous measurements at satellite sites show that the Fresno Supersite represented PM_2.5 within the city, and that half or more of the urban concentrations were present at distant, non-urban locations unaffected by local sources. Most of the primary particles accumulated during early morning and nighttime, decreasing when surface temperatures increased and the shallow radiation inversion coupled to a valleywide layer. When this coupling occurred, nitrate levels increased rapidly over a 10–30 min period as black carbon and gaseous concentrations dropped. This is consistent with a conceptual model in which secondary aerosol forms above the surface layer and is effectively decoupled from the surface for all but the late-morning and early afternoon period. Primary pollutants, such as organic and black carbon, accumulate within the shallow surface layer in urban areas where wood burning and vehicle exhaust emissions are high. Such a model would explain why earlier studies find nitrate concentrations to be nearly the same among widely separated sites in urban areas, as winds aloft of 1 to 6 m s⁻¹ could easily disperse the elevated aerosol throughout the valley.     

Seasonal characteristics of water-soluble organic carbon in atmospheric particles in the inland Kanto plain,Japan

An investigation of water-soluble organic carbon (WSOC) in atmospheric particles was conducted as an index of the formation of secondary organic aerosol (SOA) from April 2005 to March 2006 at Maebashi and Akagi located in the inland Kanto plain in Japan. Fine (<2.1 μm) and coarse (2.1–11 μm) particles were collected by using an Andersen low-volume air sampler, and WSOC, organic carbon (OC), elemental carbon (EC), and ionic components were measured. The mean mass concentrations of the fine particles were 22.2 and 10.5 μg m^?3 at Maebashi and Akagi, respectively. The WSOC in fine particles accounted for a large proportion (83%) of total WSOC. The concentration of fine WSOC ranged from 1.2 to 3.5 μg-C m^?3 at Maebashi, rising from summer to fall. At Akagi, it rose from spring to summer, associated with the southerly wind from urban areas. The WSOC/OC ratio increased in summer at both sites, but the ratio at Akagi was higher, which we attributed to differences in primary emissions and secondary formation between the sites. The fine WSOC concentration was significantly positively correlated with concentrations of SO₄^2?, EC, and K⁺, and we inferred that WSOC was produced by photochemical reaction and caused by the combustion of both fuel and biomass. We estimated that SOA accounted for 11–30% of the fine particle mass concentration in this study, suggesting that SOA is a significant year-round component in fine particles.     

On the variability of Black Smoke and carbonaceous aerosols in the Netherlands

The study addresses the characteristics of elemental carbon (EC) and organic carbon (OC) distributions in the Netherlands by using Black Smoke (BS) data in combination with dedicated measurements and modelling. The BS levels indicate a large-scale background concentration over the Netherlands with low spatial variability and a gradient with highest levels (∼9 μg m⁻³) in the south gradually decreasing to the north-west (∼5.5 μg m⁻³). The BS concentrations at rural sites in the Netherlands are highly correlated due to common (diffuse) sources and large-scale meteorology. Superimposed on the regional background are the contributions of local/urban sources. Urban and rural BS levels show a distinct variation over the week with minimum levels on Sundays.BS levels do not reflect a real concentration as they are obtained via an optical measurement in combination with an outdated calibration curve to arrive at total suspended particles (TSP). We have found that the relation between BS and EC in the Netherlands is linear and highly correlated but dependent on station type. Application of these relations to the BS time series yields a gradient in the rural background EC concentration from 0.5 μg m⁻³ in the north to 0.7 μg m⁻³ in the south of the Netherlands. The relationship between OC and BS appears to be location specific and is determined by the BS–EC relation in combination with a characteristic OC/EC ratio. OC/EC ratios are ∼5 at regional background sites and ∼2 at traffic locations. Minimum OC/EC ratios at the traffic sites reflect the primary OC/EC ratio of traffic. We argue that estimation of secondary organic aerosol by assuming the minimum OC/EC ratio to be a proxy for the primary OC/EC is not allowed since this approach does not account for sources with high OC/EC ratios. Based on European scale modelling and the measured data, we estimate that national sources contribute ∼40–60% to Dutch EC levels.The rather costly and laborious EC measurements provide a better indicator of the carbonaceous fraction in ambient particulate matter (PM) but the cheap BS method may provide valuable information on spatial distribution of EC when used in combination with validation sites to characterise the EC–BS relationship.