Characterization Of Carbonaceous Aerosols Research Articles

Characterization of carbonaceous aerosols during the Indian summer monsoon over a rain-shadow region

Characterization of carbonaceous aerosols during the Indian summer monsoon over a rain-shadow region

Characterization of carbonaceous aerosols in Singapore: insight from black carbon fragments and trace metal ions detected by a soot particle aerosol mass spectrometer

Abstract. Understanding sources and atmospheric processes that can influence the physiochemical properties of carbonaceous aerosols is essential to evaluate their impacts on air quality and climate. However, resolving the sources, emission characteristics, and aging processes of carbonaceous aerosols in complex urban environments remains challenging. In this work, a soot particle aerosol mass spectrometer (SP-AMS) was deployed to characterize organic aerosols (OAs), refractory black carbon (rBC), and trace metals in Singapore, a highly urbanized city with multiple local and regional air pollution sources in the tropical region. rBC (C1+–C9+) fragments and trace metal ions (K+, Na+, Ni+, V+, and Rb+) were integrated into our positive matrix factorization of OA. Two types of fossil fuel combustion-related OAs with different degrees of oxygenation were identified. This work provides evidence that over 90 % of rBC originated from local combustion sources with a major part related to traffic and ∼30 % associated with fresh secondary organic aerosol (SOA) produced under the influence of shipping and industrial emission activities (e.g., refineries and petrochemical plants) during daytime. The results also show that ∼43 % of the total rBC was emitted from local traffic, while the rest of the rBC fraction stemmed from multiple sources including vehicular sources, shipping, and industrial emissions, but was not fully resolved. There was only a weak association of the cooking-related OA component with rBC. Although there was no observable biomass burning episode during the sampling period, K+ and Rb+ were mainly associated with the more oxidized oxygenated OA component, indicating the potential contribution of regional biomass burning and/or coal combustion emissions to this aged OA component. Furthermore, the aerosol pollutants transported from the industrial area and shipping ports presented higher C1+/C3+ and V+/Ni+ ratios than those associated with traffic. The observed association between Na+ and rBC suggests that the contribution of anthropogenic emissions to total particulate sodium should not be ignored in coastal urban environments. Overall, this work demonstrates that rBC fragments and trace metal ions can improve our understanding of the sources, emission characteristics, and aging history of carbonaceous aerosol (OA and rBC) in this type of complex urban environment.

Characterization of carbonaceous aerosols over the Northern Adriatic Sea in the JERICO-NEXT project framework

The coastal aerosol represents a complex mixing between sea spray aerosols locally generated at the sea surface and a component generated by natural and/or anthropogenic sources on the nearby land. The aim of this paper is to study the atmospheric concentrations of carbonaceous compounds as measured in the coastal zone of the Northern Adriatic Sea between April 2017 and April 2018. The results show a quite large contribution of carbonaceous compounds, even when the sampled air mass is predominantly maritime. Although it is generally assumed that 70% and 90% of bulk organic carbon (OC) and elemental carbon (EC) concentrations, respectively, are found in the fine mode, we observed higher OC and EC concentrations in the coarse fraction (up to about 37% and 25%, respectively). This confirms the occurrence of mixing between anthropogenic matter and sea spray, mainly composed of coarse aerosol particles, during the atmospheric transport over the Mediterranean basin.

Characterization of carbonaceous aerosols in Asian outflow in the spring of 2015: Importance of non-fossil fuel sources

The sources of elemental (EC) and organic carbon (OC) aerosols in Asian outflow were investigated in the spring of 2015 in terms of radiocarbon (14C) and molecular marker analyses. The contribution of fossil fuel (FF) sources to carbonaceous aerosols (TC) significantly increased in polluted air masses with enhancements in the concentrations of carbon monoxide. For EC, FF sources dominated in the polluted air masses. For OC, the contributions of non-FF sources other than biomass burning (BB) were found to be significant (comparable to or higher than those of FF sources), especially in air masses with higher values of the water-soluble fraction of OC (fWSOC) and 14C concentrations (F14C). Positive correlations between fWSOC and F14C indicate that the origins of TC (mainly OC) have great impacts on the water solubility variability and the subsequent cloud formation processes of OC during transport. We found the importance of natural sources as possible origins of OC in non-polluted (i.e., background) air. This study raises the need to further investigate the source apportionment of OC, especially its natural origins, for more accurately assessing the climatic impacts of EC and OC in East Asia.

Use of the integrated organic gas and particle sampler to improve the characterization of carbonaceous aerosol in the near-road environment

Abstract Particle phase organic carbon (OC), elemental carbon (EC) and particle phase semi-volatile organic carbon were measured simultaneously at two distances downwind of a highway using an integrated organic gas and particle sampler. This method reduces sampling artifacts associated with OC measurement. On average, artifact-corrected OC (referred to as OC T ) was 2.4 μg/m 3 and the positive and negative artifacts were significant at 0.8 and 1.0 μg/m 3 respectively. Close to the highway negative artifacts are potentially dominant over positive artifacts indicating that traditional integrated filter-based sampling for OC and fine particles (PM 2.5 ) may be biased low. Decreases in OC T between the near and far site ranged from 25 to 44% while the decreases observed for EC, which reflects the impact of dispersion, were larger at 42–84%. The nature of the OC T changed between sites becoming less volatile and having a greater content of pyrolized organic carbon. Collectively, these results suggest that secondary organic aerosol (SOA) formed downwind of the highway from vehicle-related emissions and was detectable within the 15 min transit time between the highway and the far site. These results highlight the need for improvements in understanding the processes influencing organic aerosols in locations directly impacted by motor vehicle emissions in order to realistically predict PM 2.5 using air quality models.

Characterization of carbonaceous aerosols at Mount Lu in South China: implication for secondary organic carbon formation and long-range transport.

In order to understand the sources and potential formation processes of atmospheric carbonaceous aerosols in South China, fine particle samples were collected at a high-elevation mountain site--Mount Lu (29°35' N, 115°59' E, 1165 m A.S.L.) during August-September, 2011. Eight carbonaceous fractions from particles were resolved following the IMPROVE thermal/optical reflectance protocol. During the observation campaign, the daily concentrations of PM2.5 at Mount Lu ranged from 7.69 to 116.39 μg/m(3), with an average of 58.76 μg/m(3). The observed average organic carbon (OC) and elemental carbon (EC) concentrations in PM2.5 were 3.78 and 1.28 μg/m(3), respectively. Secondary organic carbon (SOC) concentration, estimated by EC-tracer method, was 2.07 μg/m(3) on average, accounting for 45.0% of the total OC. The enhancement of secondary organic aerosol (SOA) formation was observed during cloud/fog processing, and heterogeneous acid-catalyzed reactions may have contributed to SOA formation as well. Back trajectory analysis indicated that air masses were mainly sourced from southern China during observation period, and this air mass source was featured by highest values of OC and effective carbon ratio (ECR). Relation of carbonaceous species and principal component analysis indicated that multiple sources contributed to the carbonaceous aerosols at Mount Lu.

Characterization of carbonaceous aerosols over the East China Sea: The impact of the East Asian continental outflow

Seventy-five paired PM2.5 (aerodynamic diameter less than 2.5 μm) and TSP (total suspended particle) samples collected from a pristine island in the East China Sea (ECS) between October 2011 and August 2012 were analyzed for organic carbon (OC), elemental carbon (EC), and n-alkanes. The island lies in the pathway of continental outflow from Mainland China to the northwest Pacific Ocean driven by the East Asian Monsoon. The concentrations of OC, EC (in μg/m3), and n-alkanes (in ng/m3) were highest in winter (means: 4.7, 1.3, 140.1, respectively) and lowest in summer (means: 1.1, 0.3, 17.0, respectively). PM2.5 contained approximately 88% of the OC, 80% of the EC, and 61% of the n-alkanes in TSP. Petroleum residue was the dominant contributor to the n-alkanes. C12–C22n-alkanes with strong even-to-odd predominance observed in winter were attributed to the microbial contribution from sea spray aerosol (SSA) driven by the higher wind speed. There was a higher secondary organic carbon (SOC)/OC ratio in warm seasons (summer and fall) than that in cold seasons (spring and winter). The dominance of primary organic carbon (POC) and EC in cold seasons was possibly mainly due to the influence of the East Asian continental outflow. Three episodes of high concentrations of carbonaceous aerosols were observed, and we focused on the impact of these pollutants from East Asia on the air quality over the ECS. Carbonaceous pollutants were more concentrated in PM2.5 during the fall episode triggered by biomass burning in East China. The winter haze associated with intensive indoor heating in North China brought substantial carbonaceous pollutants, with a minor influence on their size distribution. The dust episode in spring was related to coarse particles (i.e., TSP–PM2.5), yielding a distinctly different size distribution.

Characterization of carbonaceous aerosols over the urban tropical location and a new approach to evaluate their climatic importance

Increasing emissions from fossil-fuel, biomass burning, land use changes and industrial growth have led to rapid increase in the atmospheric concentrations of carbonaceous species over many cities in India. The present paper deals with the results obtained from year long (2012–13) observations conducted at a tropical urban location, Pune in southwestern India on Organic and Elemental Carbon as well as Black Carbon; using the Sunset OCEC Analyzer and Aethalometer, respectively. The average mass concentrations of OC and EC were in the order of winter > post-monsoon > summer > monsoon. Mean annual OC/EC ratio was found to be 2.4 ± 1.1 during the study period, suggesting the presence of secondary organic carbon (SOC). Estimated SOC was found to form 47% of OC mass concentration. OC and EC were also significantly well correlated (r = 0.95, p < 0.0001) to each other, indicating towards common combustion sources. The primary organic carbon (POC) dominated over SOC and EC in post-monsoon and winter seasons indicating impact of anthropogenic burning activity, enhanced by prevailing meteorological conditions as well as that of long range transport. Mean annual POC + EC/TC ratio was 0.69 indicating that more than 2/3 of TC is formed from combustion sources. Thermally derived EC and optically derived BC correlated very well (r = 0.98, p < 0.0001). A new concept e.g. Effective carbon ratio (ECR) is suggested to better assess the scattering/absorptive nature and probable source identification of carbonaceous aerosols in place of conventional OC/EC ratio.

Characterization of carbonaceous aerosols over Delhi in Ganga basin: seasonal variability and possible sources.

The mass concentration of carbonaceous species, organic carbon (OC), and elemental carbon (EC) using a semicontinuous thermo-optical EC-OC analyzer, and black carbon (BC) using an Aethalometer were measured simultaneously at an urban mega city Delhi in Ganga basin from January 2011 to May 2012. The concentrations of OC, EC, and BC exhibit seasonal variability, and their concentrations were ∼2 times higher during winter (OC 38.1 ± 17.9 μg m(-3), EC 15.8 ± 7.3 μg m(-3), and BC 10.1 ± 5.3 μg m(-3)) compared to those in summer (OC 14.1 ± 4.3 μg m(-3), EC 7.5 ± 1.5 μg m(-3), and BC 4.9 ± 1.5 μg m(-3)). A significant correlation between OC and EC (R = 0.95, n = 232) indicate their common emission sources with relatively lower OC/EC ratio (range 1.0-3.6, mean 2.2 ± 0.5) suggests fossil fuel emission as a major source of carbonaceous aerosols over the station. On average, mass concentration of EC was found to be ∼38 % higher than BC during the study period. The measured absorption coefficient (babs) was significantly correlated with EC, suggesting EC as a major absorbing species in ambient aerosols at Delhi. Furthermore, the estimated mass absorption efficiency (σabs) values are similar during winter (5.0 ± 1.5 m(2) g(-1)) and summer (4.8 ± 2.8 m(2) g(-1)). Significantly high aerosol loading of carbonaceous species emphasize an urgent need to focus on air quality management and proper impact assessment on health perspective in these regions.

Characterization of carbonaceous aerosols with special reference to episodic events at Agra, India

A continuous measurement of organic carbon (OC) and elemental carbon (EC) in PM2.5 and TSP was carried out at a suburban site of North central region of India. PM2.5 and TSP samples were collected from May 2010 to April 2011 and were analyzed for OC and EC using thermal optical transmittance (TOT) protocol. The results showed that the annual average concentrations of PM2.5 and TSP were 79.7±40.5 and 247.5±128.3μg/m3, respectively. In PM2.5, OC and EC concentrations were 22.8±17.1 and 3.4±1.2μg/m3 while in TSP the concentrations were 42.1±22.6 and 6.1±3.2μg/m3 respectively. Both OC and EC exhibited a clear seasonal pattern with highest concentration observed in winter followed by summer and monsoon which may be due to the combined effect of changes in emission rates and different meteorology in various seasons. Diurnal variation indicated higher concentration during night in all seasons. TCA (Total carbonaceous aerosol) accounted for an averaged 50.3% of PM2.5 mass and 29.6% of TSP mass. The annual average OC/EC ratio was 6.6 which is similar ratio for biomass burning emissions. The SOC concentrations were found to be higher during winter season in both PM2.5 and TSP. To study the influence of natural singular events in aerosol composition, three types of episodic events have been identified. The SEM/EDX analysis revealed the dominance of carbonaceous particles during winter season which is also supported by back trajectory analysis which shows that the origin of these particles is mainly anthropogenic in nature.

Characterization of carbonaceous aerosol by the stepwise-extraction thermal–optical-transmittance (SE-TOT) method

Carbonaceous aerosol collected in Beijing, China was characterized by a stepwise-extraction thermal–optical-transmittance (SE-TOT) method which allows for a quantitative separation of organic aerosol into distinct fractions. About 55% of the total organic carbon (OC) could be extracted by a mixture of hexane, methylene chloride and acetone. The extractable OC was further isolated into non-polar, low-polar and high-polar OC which constituted 10%, 23% and 22% of the total OC, respectively. The sum of low-polar and high-polar OC was found to coincide well with the secondary OC predicted by the elemental carbon tracer method, indicating that the low-polar and high-polar OC are strongly associated with secondary organic aerosol. Moreover, it was suggested that high relative humidity could enhance the production of high-polar OC through aqueous-phase reactions, because high-polar OC correlated strongly with oxalate and the ratio of high-polar OC to low-polar OC was significantly higher during the sampling events with high relative humidity (1.23 ± 0.35) comparing with results from the low relative humidity days (0.79 ± 0.23). In addition, the extractable OC was shown to be light-absorbing. The results of this study suggest that the SE-TOT method could provide new insights into the characterization of carbonaceous aerosol.

Chemical characteristics of carbonaceous aerosols during dust storms over Xi’an in China

Characterization of carbonaceous aerosols including CC (carbonate carbon), OC (organic carbon), and EC (elemental carbon) were investigated at Xi’an, China, near Asian dust source regions in spring 2002. OC varied between 8.2 and 63.7 µg m−3, while EC ranged between 2.4 and 17.2 µ m−3 during the observation period. OC variations followed a similar pattern to EC and the correlation coefficient between OC and EC is 0.89 (n=31). The average percentage of total carbon (TC, sum of CC, OC, and EC) in PM2.5 during dust storm (DS) events was 13.6%, which is lower than that during non-dust storm (NDS) periods (22.7%). CC, OC, and EC accounted for 12.9%, 70.7%, and 16.4% of TC during DS events, respectively. The average ratio of OC/EC was 5.0 in DS events and 3.3 in NDS periods. The OC-EC correlation (R2=0.76, n=6) was good in DS events, while it was stronger (R2=0.90, n=25) in NDS periods. The percentage of water-soluble OC (WSOC) in TC accounted for 15.7%, and varied between 13.3% and 22.3% during DS events. The distribution of eight carbon fractions indicated that local emissions such as motor vehicle exhaust were the dominant contributors to carbonaceous particles. During DS events, soil dust dominated the chemical composition, contributing 69% to the PM2.5 mass, followed by organic matter (12.8%), sulfate (4%), EC (2.2%), and chloride (1.6%). Consequently, CC was mainly entrained by Asian dust. However, even in the atmosphere near Asian dust source regions, OC and EC in atmospheric dust were controlled by local emission rather than the transport of Asian dust.

Characterization of carbonaceous aerosols in urban air

Concentrations of black carbon, [BC], were determined with an Aethalometer every 5 min at Lahore, a city of about 10 million in Pakistan, from 22 November 2005 to 31 January 2006. [BC] were very high, ranging from about 5 to 110 μ g m - 3 , with a mean of 21.7 μ g m - 3 . A distinct diurnal variation was observed: concentrations were lowest from about 10 a.m. to 4 p.m. local time (LT), and highest around 5–9 p.m. No clear relationship was observed between surface wind directions and [BC], although some of the highest concentrations were observed when the airflow was from southwest to northwest. The daily variations in concentrations were strongly affected by the diurnal variations in the mixing height; BC concentrations were low during the day when the mixing heights were high, ∼ 1000 m , and very high at night when the mixing heights were low < 250 m . Periods of light to dense fog occurred from 22 December through 4 January. [BC] were generally lower than average when fog occurred during the night and early morning, but they were not necessarily lower during daytime fogs. We also collected aerosols on quartz filters every 3, 6, or 12 h and determined the concentrations of elemental, [EC], and organic carbon, [OC], using the thermal–optical method. The [BC] were highly correlated with EC ( r 2 = 0.71 ) , but on average 25% higher than [EC]. The [EC] and [OC] concentrations were moderately correlated ( r 2 = 0.65 ) . The [OC]/[EC] ratios varied from 2.8 to 12, with a mean of 5.6. Although a large component of the carbonaceous aerosols in Lahore originated from fossil fuel combustion, a significant fraction was derived from biomass burning.

Characterization of carbonaceous aerosols during the MINOS campaign in Crete, July–August 2001: a multi-analytical approach

Abstract. During the major part of the Mediterranean Intensive Oxidant Study (MINOS) campaign (summer 2001, Crete Isl.), the Marine Boundary Layer (MBL) air was influenced by long range transport of biomass burning from the northern and western part of the Black Sea. During this campaign, carbonaceous aerosols were collected on quartz filters at a Free Tropospheric (FT) site, and at a MBL site together with size-resolved distribution of aerosols. Three Evolution Gas Analysis (EGA) protocols have been tested in order to better characterize the collected aged biomass burning smoke: A 2-step thermal method (Cachier et al., 1989) and a thermo-optical technique using two different temperature programs. The later temperature programs are those used for IMPROVE (Interagency Monitoring of Protected Visual Environments) and NIOSH 5040 (National Institute of Occupational Safety and Health). Artifacts were observed using the NIOSH temperature program and identified as interactions between carbon and dust deposited on the filter matrix at high temperature (T&gt;550ºC) under the pure helium step of the analysis. During the MINOS campaign, Black Carbon (BC) and Organic Carbon (OC) mass concentrations were on average respectively 1.19±0.56 and 3.62±1.08 mgC/m3 for the IMPROVE temperature program, and 1.09±0.36 and 3.75±1.24 mgC/m3 for the thermal method. Though these values compare well on average and the agreement between the Total Carbon (TC) measurements sample to sample was excellent (slope=1.00, r2=0.93, n=56), important discrepancies were observed in determining BC concentrations from these two methods (average error of 33±22%). BC from the IMPROVE temperature program compared well with non-sea-salt potassium (nss-K) pointing out an optical sensitivity to biomass burning. On the other hand, BC from the thermal method showed a better agreement with non-sea-salt sulfate (nss-SO4), considered as a tracer for fossil fuel combustion during the MINOS campaign. The coupling between these two methods for determining BC brings here new insights on the origin of carbonaceous aerosols in a complex mixture of different sources. It brings also to our attention that important deviations in BC levels are observed using three widely used EGA's techniques and most probably none of the EGA tested here are well adapted to fully characterize this aerosol mixture. Spherical, smooth and silico-aluminated fly-ash observed by an Analytical Scanning Electron Microscope (ASEM) confirm the influence of coal combustion on the carbonaceous aerosol load throughout the campaign. A rough calculation based on a BC/nss-SO4 mass ratio suggests that biomass burning could be responsible for half of the BC concentration recorded during the MINOS campaign. From the plot of BC as a function of TC, two linear correlations were observed corresponding to 2 times series (before and after 12 August). Such good correlations suggest, from a first look, that both BC and OC have similar origin and atmospheric transport. On the other hand, the plot of BC as a function of TC obtained from the 2-step thermal method applied to DEKATI Low Pressure Cascade Impactor samples does not show a similar correlation and points out a non conservative distribution of this ratio with 2 super micron modes enriched in OC, correlated with sea salt aerosols and probably originating from gas-to-particle conversion.

Characterization of carbonaceous aerosols in China

Characterization of carbonaceous aerosols in China

Characterization of carbonaceous aerosols in the Nagoya urban area. 2. Behavior and origin of particulate n-alkanes

Measurements of concentrations, size distributions, and vapor-to-particle partitioning for n-alkanes in ambient aerosol were made in the Nagoya urban area. The average concentration of total particulate n-alkanes in the winter was roughly 5 times higher to that in the summer. The distribution profiles of particular n-alkanes in the summer showed a saw-tooth pattern (odd>even) in the range CZ 7 -C 35 . Ont the other hand, in the winter a nearly Gaussian distribution with a maximum around C 22 overlapped with the saw-tooth pattern. It was found that a major cause of the seasonal changes in the lower n-alkanes of the distribution profiles is not a change in fossil fuel emissions, but rather vapor-to-particle partitioning

Characterization of carbonaceous aerosols in the Nagoya urban area. 1. Elemental and organic carbon concentrations and the origin of organic aerosols

Determination des concentrations en carbone elementaire et en carbone organique dans des echantillons d'air collectes dans la zone urbaine de Nagoya