Thermal-optical Method Research Articles

Measured black carbon deposition over the central Himalayan glaciers: Concentrations in surface snow and impact on snow albedo reduction

Deposition of ambient black carbon (BC) aerosols over snow-covered areas reduces surface albedo and accelerates snowmelt. Based on in-situ atmospheric BC data and the WRF-Chem model, we estimated the dry and wet deposition of BC over the Yala glacier of the central Himalayan region in Nepal during 2016–2018. The maximum and minimum BC dry deposition was reported in pre- and post-monsoon respectively. Approximately 50% of annual dry deposition occurred in the pre-monsoon season (March to May) and 27% of the annual dry deposition occurred in April. The total dry BC deposition rate was estimated as ∼4.6 μg m−2 day−1 providing a total deposition of 531 μg m−2 during the pre-monsoon season. The contribution of biomass burning and fossil fuel sources to BC deposition on an annual basis was 28% and 72% respectively. The annual accumulated wet deposition of BC was 196 times higher than the annual dry deposition. The ten months of observed dry deposition of BC (October 1, 2016 to August 31, 2017 – except December 2016) was ∼39% lower than that of WRF-Chem's estimated annual dry deposition from September 1, 2016 to August 31, 2017 partially due to model bias. The deposited content of BC over the snow surface has an important role in albedo reduction, therefore snow samples were collected from the surface of the Yala Glacier and the surrounding region in April 2016, 2017, and 2018. Samples were analyzed for BC mass concentration through the thermal optical analysis and single particle soot photometer method. The BC calculated via the thermal optical method was in the range of 352–854 ng g−1, higher than the BC calculated through the particle soot photometer method and estimated BC in 2 cm surface snow (imperial equation). The maximum surface snow albedo reduction due to BC was 8.8%, estimated by a widely used snow radiative transfer model and a linear regression equation.

Evaluation of a non-dispersive infrared spectrometer for quantifying organic and elemental carbon in diesel particulate matter.

Diesel particulate matter (DPM) is a common and well-known health hazard in the mining environment. The regulatory method for monitoring both the organic and elemental carbon (OC, EC) portions of DPM is a laboratory-based thermal-optical method with a typical turnaround time of one week. In order to evaluate exposure levels and take corrective action prior to overexposure, a portable real-time device capable of quantifying both OC and EC is needed. To that end, researchers from the National Institute for Occupational Safety and Health (NIOSH) designed and tested the feasibility of a device based on bandpass optical filters that target key infrared wavelengths associated with DPM and its spectroscopic baseline. The resulting device, referred to here as a non-dispersive infrared (NDIR) spectrometer could serve as the basis of a cost-effective, field-portable alternative to the laboratory thermal-optical method. The limits of quantification (LOD) indicate that the NDIR spectrometer can quantify EC, OC, and TC provided they are present at 20, 37, and 46 μg/m3 or more, respectively. In the event that the NDIR spectrometer is integrated with a sampler and filter tape the LOD is estimated to be reduced to 13, 7, and 10 μg/m3 for EC, OC, and TC, respectively. These LOD estimates assume a face velocity of 59 cm/s and a sampling time of 30 min.

Black carbon: a general review of its sources, analytical methods, and environmental effects in snow and ice in the Tibetan Plateau.

Tibetan Plateau (TP) is known as the water tower of Asia, and glaciers are solid reservoirs that can regulate the amount of water. Black carbon (BC), as one of the important factors accelerating glacier melting, is causing evident environmental effects in snow and ice. However, a systematical summary of the potential sources, analytical methods, distributions, and environmental effects of BC in snow and ice on the TP's glaciers is scarce. Therefore, this study drew upon existing research on snow and ice BC on glaciers of the TP to describe the detection methods and uncertainties associated with them to clarify the concentrations of BC in snow and ice and their climatic effects. The primary detection methods are the optical method, the thermal-optical method, the thermochemical method, and the single-particle soot photometer method. However, few studies have systematically compared the results of BC and this study found that concentrations of BC in different types of snow and ice varied by 1-3 orders of magnitude, which drastically affected the regional hydrologic process by potentially accelerating the ablation of glaciers by approximately 15% and reducing the duration of snow accumulation by 3-4 days. In general, results obtained from the various testing methods differ drastically, which limited the systematical discussion. Accordingly, a universal standard for the sampling and measurement should be considered in the future work, which will be beneficial to facilitate the comparison of the spatiotemporal features and to provide scientific data for the model-simulated climatic effects of BC.

Distribution characteristics and optical properties of carbonaceous aerosol: brown carbon and black carbon in Nanchang, inland China

PM2.5 samples were collected from October 31, 2019, to November 10, 2019, in Nanchang for 10 consecutive days. The mass concentrations of PM2.5 and carbon components were measured, and the distribution characteristics of carbonaceous aerosols were discussed. The optical properties of carbonaceous aerosols were quantified by the thermal-optical method and solvent extraction method, respectively. The results showed that the average concentrations of organic carbon (OC) and elemental carbon (EC) in aerosols in Nanchang were 11.79 ± 3.86 and 3.51 ± 1.59 μg m−3, respectively. The average OC/EC was 3.62, and OC2, OC3, OC4 and EC1 accounted for relatively large proportions (19.55, 24.96, 22.37 and 17.38%). Carbonaceous aerosols in Nanchang were greatly affected by coal combustion, vehicle exhaust emissions and secondary organic carbon (SOC) formation. For particulate brown carbon (BrC), the average light absorption coefficient (babs) and mass absorption efficiency (MAE) at 405 nm were 16.87 Mm−1 and 1.49 m2g−1, respectively. The average Absorption Ångström exponent (AAE) was 8.58. For water-soluble organic carbon (WSOC) and methanol-soluble organic carbon (MSOC), the average babs,365,WSOC and babs,365,MSOC were 14.79 and 22.51 Mm−1, respectively. The mean values of AAE300-600,WSOC and AAE300-600,MSOC were 4.17 and 4.84, respectively. The mean MAE365,WSOC and MAE365,MSOC were 1.83 and 2.18 m2 g−1, respectively. The mean value of MAEBC at 405 nm was 10.28 m2 g−1. The optical properties of particulate BrC and dissolved BrC were similar at 405 nm. The light absorption of BrC cannot be ignored, although BC was the main light absorption component.

Significant overestimation of black carbon concentration caused by high organic carbon in aerosols of the Tibetan Plateau

Black carbon plays an important role in climate change. Whereas, accurate measurement of black carbon (also known as elemental carbon (EC)) is still a challenging issue because portion of the pyrolytic carbon produced from the organic carbon (OC) can cause the overestimation of EC when measured by thermal-optical method. As one of the remote regions in the world, the Tibetan Plateau (TP) is characterized as high OC/EC ratio in its atmosphere. In this study, potential influence of relative high OC concentration to EC were investigated at three remote sites (Yaze, Everest and Nam Co) in the TP. The results showed that carbonaceous aerosols from different sources can affect the fraction of OC extracted by methanol. Concentration of OC extracted by methanol had a significantly positive correlation with the reduction of pyrolytic carbon and EC concentrations, indicating that part of OC extracted by methanol can decrease the production of pyrolytic carbon and then reduce the overestimation of EC. After considering this effect, it is shown in this study that actual EC concentration at Yaze, Everest and Nam Co were overestimated by approximately 40.0 ± 12.6%, 28.8 ± 9.1% and 24.8 ± 4.7%, respectively. Accordingly, combined with the overestimation of EC concentration by carbonates, actual ratios of solar energy absorbed by organic carbon to EC were 1.67, 2.33 and 2.78 times those of original ones at Yaze, Everest and Nam Co, respectively. Therefore, warming effect caused by EC on the TP should be lower than that previously estimated. This phenomenon needs to be considered for both in situ study and model simulation in the future.

Characteristics of wintertime carbonaceous aerosols in two typical cities in Beijing-Tianjin-Hebei region, China: Insights from multiyear measurements

In order to investigate the impact of “Blue Sky War” implemented during 2018–2020 on carbonaceous aerosols in Beijing-Tianjin-Hebei (BTH) region, China, fine particulate matter (PM2.5) samples were collected simultaneously in Tianjin and Handan in three consecutive winters from 2018 to 2020. Organic carbon (OC) and elemental carbon (EC) in PM2.5 were measured with the same thermal-optical methods and analysis protocols. Significant reductions in primary organic carbon (POC) and EC concentrations were observed both in Tianjin and Handan, with decreasing rates of 0.65 and 2.95 μg m−3 yr−1 for POC and 0.13 and 0.64 μg m−3 yr−1 for EC, respectively. The measured absorption coefficients of EC (babs, EC) also decreased year by year, with a decreasing rate of 1.82 and 6.16 Mm−1 yr−1 in Tianjin and Handan, respectively. The estimated secondary organic carbon (SOC) concentrations decreased first and then increased in both Tianjin and Handan, accounting for more than half of the total OC in winter of 2020–2021 and with increasing contributions especially in highly polluted days. SOC was recognized as one of key factors influencing EC light absorption. EC in the two cities was relatively more related to coal combustion and industrial sources. The reductions of primary carbonaceous components may be attributed to the air quality regulations targeting coal combustion and industrial sources emissions in BTH area. Potential source contribution function (PSCF) analysis results indicated that the major source areas of OC and EC in Tianjin were the southwest region of the sampling site, while the southeast areas for Handan. These findings demonstrated the effectiveness of air quality regulation in primary emissions in typical polluted cities in BTH region and highlighted the needs for further control and in-depth investigation of SOC formation along with implementation of air pollution control act in the future.

Measurement of light-absorbing particles in surface snow of central and western Himalayan glaciers: spatial variability, radiative impacts, and potential source regions

Abstract. We collected surface snow samples from three different glaciers – Yala, Thana, and Sachin – in the central and western Himalayas to understand the spatial variability and radiative impacts of light-absorbing particles. The Yala and Thana glaciers in Nepal and Bhutan, respectively, were selected to represent the central Himalayas. The Sachin glacier in Pakistan was selected to represent the western Himalayas. The samples were collected during the pre- and post-monsoon seasons of the year 2016. The samples were analyzed for black carbon (BC) and water-insoluble organic carbon (OC) through the thermal optical method. The average mass concentrations (BC 2381 ng g−1; OC 3896 ng g−1; dust 101 µg g−1) in the western Himalayas (Sachin glacier) were quite high compared to the mass concentrations (BC 358 ng g−1, OC 904 ng g−1, dust 22 µg g−1) in the central Himalayas (Yala glacier). The difference in mass concentration may be due to the difference in elevation, snow age, local pollution sources, and meteorological conditions. BC in surface snow was also estimated through Weather Research and Forecasting (WRF) model coupled with Chemistry (WRF-Chem) simulations at the three glacier sites during the sampling periods. Simulations reasonably capture the spatial and seasonal patterns of the observed BC in snow but with a relatively smaller magnitude. Absolute snow albedo was estimated through the Snow, Ice, and Aerosol Radiative (SNICAR) model. The absolute snow albedo reduction ranged from 0.48 % (Thana glacier during September) to 24 % (Sachin glacier during May) due to BC and 0.13 % (Yala glacier during September) to 5 % (Sachin glacier during May) due to dust. The instantaneous radiative forcing due to BC and dust was estimated in the range of 0 to 96.48 and 0 to 25 W m−2, respectively. The lowest and highest albedo reduction and radiative forcing were observed in central and western Himalayan glaciers, respectively. The potential source regions of the deposited pollutants were inferred using WRF-Chem tagged-tracer simulations. Selected glaciers in the western Himalayas were mostly affected by long-range transport from the Middle East and central Asia; however, the central Himalayan glaciers were mainly affected by local and south Asia emissions (from Nepal, India, and China) especially during the pre-monsoon season. Overall, south Asia and west Asia were the main contributing source regions of pollutants.

Experimental Characterization of PM2.5 Organic Carbon by Using Carbon-fraction Profiles of Organic Materials

Organic aerosols (OA) in the atmosphere have complex emission sources and formation processes that must be determined to understand the OA composition and behavior. The thermal optical method is generally used to analyze organic carbon (OC) in OAs, and the resulting thermally fractionated OC profiles can be considered to be a synthesis of the organic materials contained in OAs. In this study, carbon-fraction profiles of 43 organic materials were determined and categorized into five types on the basis of their profile patterns. Then a chemical mass balance (CMB) analysis using the five types and the measured carbon-fraction profiles of particulate OC from various emission sources was conducted. The major sources thus determined were generally reasonable considering the known chemical properties of emission source particles. In addition, the seasonal organic matter composition in ambient particulate OC measured at a suburban site of Tokyo was experimentally estimated by a CMB analysis using the five types, and the potential of making good use of thermally fractionated OC data to understand the characteristics of OAs was discussed.

Intercomparison Experiment of Water-Insoluble Carbonaceous Particles in Snow in a High-Mountain Environment (1598 m a.s.l.)

The harmonization of sampling, sample preparation and laboratory analysis methods to detect carbon compounds in snow requires detailed documentation of those methods and their uncertainties. Moreover, intercomparison experiments are needed to reveal differences and quantify the uncertainties further. Here, we document our sampling, filtering, and analysis protocols used in the intercomparison experiment from three laboratories to detect water-insoluble carbon in seasonal surface snow in the high-mountain environment at Kolm Saigurn (47.067842° N, 12.98394° E, alt 1598 m a.s.l.), Austria. The participating laboratories were TU Wien (Austria), the University of Florence (Italy), and the Finnish Meteorological Institute (Finland). For the carbon analysis, the NIOSH5040 and EUSAAR2 protocols of the OCEC thermal-optical method were used. The median of the measured concentrations of total carbon (TC) was 323 ppb, organic carbon (OC) 308 ppb, and elemental carbon (EC) 16 ppb. The methods and protocols used in this experiment did not reveal large differences between the laboratories, and the TC, OC, and EC values of four inter-comparison locations, five meters apart, did not show meter-scale horizontal variability in surface snow. The results suggest that the presented methods are applicable for future research and monitoring of carbonaceous particles in snow. Moreover, a recommendation on the key parameters that an intercomparison experiment participant should be asked for is presented to help future investigations on carbonaceous particles in snow. The work contributes to the harmonization of the methods for measuring the snow chemistry of seasonal snow deposited on the ground.

Intercomparison of equivalent black carbon (eBC) and elemental carbon (EC) concentrations with three-year continuous measurement in Beijing, China

Due to the lack of black carbon (BC) measurement data in some cases, elemental carbon (EC) is often used as a surrogate of BC, with a simple assumption that they are interchangeable. Such assumption will inevitably lead to uncertainties in radiative forcing estimation and health impact assessment. In order to quantitatively and systematically evaluate the relationship between BC and EC as well as factors responsible for their difference, 3-year collocated equivalent BC (eBC) and EC measurements with 1-h resolution were performed in Beijing, China continuously from 2016 to 2019. EBC concentration was measured by the multi-wavelength aethalometer (AE-33) based on optical analysis, while EC concentration was determined by semi-continuous OC/EC analyzer with thermal-optical method. The results showed that around 90% of eBC concentration was higher than that of EC, with average difference between eBC and EC as 1.21 μg m−3 (accounting for 33% of average eBC in Beijing). EBC and EC concentrations exhibited strong correlation (r = 0.90) during the whole study period, but the slopes (or eBC/EC ratio) and correlation coefficients varied across seasons (spring: 1.67 and 0.94; summer: 0.91 and 0.65; fall: 1.15 and 0.88; winter: 1.09 and 0.91, respectively). Based on the information from shell/core ratios by Single Particle Soot Photometer (SP2), source apportionment results by positive matrix factorization model, and chemical composition of PM2.5, the differences between eBC and EC concentrations were found to be primarily related to BC aging process and secondary components as evidenced by strong positive correlation with secondary species (e.g., secondary organic carbon and nitrate). This study provided seasonal specific conversion factors of eBC and EC in Beijing and helpful reference for other areas, which will contribute new knowledge of carbonaceous aerosol and reduce uncertainty in assessing future climate change and health studies of BC.

Contribution of coal combustion to black carbon: Coupling tracers with the aethalometer model

Black carbon (BC) aerosol characteristics have been analysed from January 2016 to March 2017 in an urban background area (León, Spain), located in a coal-mining region, where this fuel is commonly used. The monthly and seasonal variations of BC and source contributions were examined. The mean equivalent BC concentration (eBC) during cold and warm months were 1.0 ± 0.5 and 0.6 ± 0.2 μg m−3, respectively. eBC can be further divided into eBCff (eBC from liquid fossil fuel) and eBCbb+cc (eBC from biomass burning plus coal combustion), with mean annual values of 0.6 ± 0.3 and 0.3 ± 0.3 μg m−3 (cold months) and 0.4 ± 0.2 μg m−3 and 0.1 ± 0.1 μg m−3 (warm months), respectively. The eBC obtained from the aethalometer and the elemental carbon (EC) quantified through a Thermal Optical Transmittance method presented a significant strong positive correlation in both warm (r = 0.82) and cold (r = 0.88) periods. A mass absorption cross-section (MAC) of 4.46 ± 0.16 between two techniques has been obtained. In the cold period, a multilinear regression model to decouple eBCbb from eBCcc was established (r2 = 0.85) based on two tracers: arsenic for coal combustion and potassium for biomass burning. The model application enabled us to distinguish the contributions to eBCbb+cc (as a function of the variance explained by the tracers) in the cold period: 74% from biomass burning and 26% from coal combustion. The highest eBCcc concentration was estimated for December 2016 and January 2017 (0.18 μg m−3). This result was supported by the Absorption Ångström Exponent (AAE), which showed the maximum value in January 2017 (1.43 ± 0.37) due to the high biomass burning and coal combustion contributions.

13C signatures of aerosol organic and elemental carbon from major combustion sources in China compared to worldwide estimates

Carbon isotope signatures are used to gain insight into sources and atmospheric processing of carbonaceous aerosols. Since elemental carbon (EC) is chemically stable, it is possible to apportion the main sources of EC (C3/C4 plant burning, coal combustion, and traffic emissions) using a dual 14C-13C isotope approach. The dual-isotope source apportionment crucially relies on accurate knowledge of 13C source signatures, which are seldom measured for EC. In this work, we present 13C signatures of organic carbon (OC) and EC for relevant sources in China. EC was isolated for 13C analysis based on the OC/EC split point of a thermal-optical method (EUSAAR_2 protocol). A series of sensitivity studies were conducted to investigate the EC separation and the relationship of the thermal-optical method to other EC isolation methods. Our results show that, first, the 13C signatures of raw materials and EC related to traffic emissions can be separated into three groups according to geographical location. Second, the 13C signature of OC emitted by the flaming combustion of C4 plants is strongly depleted in 13C compared to the source materials, and therefore EC is a better tracer for this source than total carbon (TC). A comprehensive literature review of 13C source signatures (of raw materials, of TC, and of EC isolated using a variety of thermal methods) was conducted. Accordingly, we recommend composite 13C source signatures of EC with uncertainties and detailed application conditions. Using these source signatures of EC in an example dual-isotope source apportionment study shows an improvement in precision. In addition, 13C signatures of OC were measured at three different desorption temperatures roughly corresponding to semi-volatile, low-volatile, and non-volatile OC fractions. Each source category shows a characteristic trend of 13C signatures with desorption temperature, which is likely related to different OC formation processes during combustion.

An automated method for thermal-optical separation of aerosol organic/elemental carbon for 13C analysis at the sub-μgC level: A comprehensive assessment

We describe and thoroughly evaluate a method for 13C analysis in different fractions of carbonaceous aerosols, especially elemental carbon (EC). This method combines a Sunset thermal-optical analyzer and an isotope ratio mass spectrometer (IRMS) via a custom-built automated separation, purification, and injection system. Organic carbon (OC), EC, and other specific fractions from aerosol filter samples can be separated and analyzed automatically for 13C based on thermal-optical protocols (EUSAAR_2 in this study) at sub-μgC levels. The main challenges in isolating EC for 13C analysis are the possible artifacts during OC/EC separation, including the premature loss of EC and the formation of pyrolyzed OC (pOC) that is difficult to separate from EC. Since those artifacts can be accompanied with isotope fractionation, their influence on the stable isotopic composition of EC was comprehensively investigated with various test compounds. The results show that the thermal-optical method is relatively successful in OC/EC separation for 13C analysis. The method was further tested on real aerosols samples. For biomass-burning source samples, (partial) inclusion of pOC into EC has negligible influence on the 13C signature of EC. However, for ambient samples, the influence of pOC on the 13C signature of EC can be significant, if it is not well separated from EC, which is true for many current methods for measuring 13C on EC. A case study in Xi'an, China, where pOC is enriched in 13C compared to EC, shows that this can lead to an overestimate of coal and an underestimate of traffic emissions in isotope-based source apportionment.

Characterisation of Atmospheric Particulate Matter from Opencast Coal Mining Activities and Adjacent Communities

Standard source apportionment techniques for atmospheric particulate (PM) collected near opencast coal mines provide less accurate results, as the inorganic mineral components in the overburden and at adjacent residential locations are similar. This study explores the use of the stable carbon (C) and nitrogen (N) isotope ratios (13C/12C and 15N/14N) and thermal optical methods to differentiate sources of carbonaceous material in the atmospheric PM samples from the opencast coal mines and adjacent communities. Both techniques allow a clear distinction between atmospheric PM samples from the opencast coal mines and communities to be made, although distinguishing between the contributions of coal combustion, liquid fuel combustion and the domestic use of biomass for requires further analysis.

Exposure assessment of elemental carbon, polycyclic aromatic hydrocarbons and crystalline silica at the underground excavation sites for top-down construction buildings.

Enclosed underground excavation worksite has an environment with poor ventilation and exposure to hazardous substances from diesel engine exhaust and construction materials. The objective of this study was to evaluate the exposure level of elemental carbon (EC), organic carbon (OC), total carbon (TC), polycyclic aromatic hydrocarbons (PAHs), dust and crystalline silica (CS) during underground excavation work for top down construction buildings. Active local air sampling for EC, OC, and TC (n = 105), PAHs (n = 50), dust (n = 34) and CS (n = 34) was conducted from inside and outside the excavator at underground excavation workshop in four different construction sites. EC, OC, TC and CS were sampled with each respirable and total particulates. EC, OC, and TC were collected on quartz-filter and analyzed using the thermal optical transmittance method. PAHs was collected on polytetrafluorethylene filter with XAD-2 and analyzed using liquid chromatography with fluorescence detector. CS and particulates were collected on poly vinyl chloride filter and analyzed using fourier-transform infrared spectroscopy. The geometric mean of respirable EC, OC, TC, total PAHs, respirable dust and respirable CS were 8.69 μg/m3, 34.32 μg/m3, 44.96 μg/m3, 6.818 μg/m3 0.13 mg/m3 and 0.02 mg/m3 from inside the excavator and 33.20 μg/m3, 46.53 μg/m3, 78.21 μg/m3, 3.934 μg/m3, 0.9 mg/m3 and 0.08 mg/m3 from outside the excavator (underground excavation workshop), respectively. The EC and RCS concentration from outside the excavator is significantly higher than that of inside the excavator (p<0.01). The worksite with rock ground, higher vehicle density, blasting and enclosed environments had higher exposure to EC than other sites (p<0.05). There was no significant difference of EC concentration between total and respirable particulates. In top down construction sites, EC concentrations during underground excavation work exceeded recommended exposure limits as 20 μg/m3, accounted for about 50% of the total sample, and the level of concentration of RCS exceeded 1.5 times of occupational exposure limit, 0.05 mg/m3. Efforts are needed to minimize exposure to diesel engine exhaust and silica in underground excavation sites. Management of diesel engine vehicle, supply of fresh air and ventilation and introducing water facilities to create wet environment in underground worksites are strongly suggested.

Sampling, Filtering, and Analysis Protocols to Detect Black Carbon, Organic Carbon, and Total Carbon in Seasonal Surface Snow in an Urban Background and Arctic Finland (&gt;60° N)

Black carbon (BC), organic carbon (OC), and total carbon (TC) in snow are important for their climatic and cryospheric effects. They are also part of the global carbon cycle. Atmospheric black and organic carbon (including brown carbon) may deposit and darken snow surfaces. Currently, there are no standardized methods for sampling, filtering, and analysis protocols to detect carbon in snow. Here, we describe our current methods and protocols to detect carbon in seasonal snow using the OCEC thermal optical method, a European standard for atmospheric elemental carbon (EC). We analyzed snow collected within and around the urban background SMEARIII (Station for Measuring Ecosystem-Atmosphere Relations) at Kumpula (60° N) and the Arctic GAW (Global Atmospheric Watch) station at Sodankylä (67° N). The median BC, OC, and TC in snow samples (ntot = 30) in Kumpula were 1118, 5279, and 6396 ppb, and in Sodankylä, they were 19, 1751, and 629 ppb. Laboratory experiments showed that error due to carbon attached to a sampling bag (n = 11) was &lt;0.01%. Sonication slightly increased the measured EC, while wetting the filter or filtering the wrong side up indicated a possible sample loss. Finally, we discuss the benefits and drawbacks of OCEC to detect carbon in snow.

Characteristics of Carbonaceous Matter in Aerosol from Selected Urban and Rural Areas of Southern Poland

The purpose of this study is to obtain a detailed picture of the spatial and seasonal variability of carbonaceous matter in southern Poland. Particulate matter (PM) samples from eight selected urban and rural background sites were analyzed for organic carbon (OC) and elemental carbon (EC) (thermal-optical method, “eusaar_2” protocol), and the content of secondary (SOC) and primary organic carbon (POC) was estimated. The OC and EC dynamics were further studied using each of the thermally-derived carbon fractions (OC1–4, PC, and EC1–4). Clear spatiotemporal variability of carbonaceous compounds concentrations was observed, with higher levels recorded during the heating season. The considered measurement sites differed particularly in the shares of SOC and POC, with higher values of POC contents especially in rural areas. In terms of the content of carbon fractions, the analyzed sites showed roughly the same characteristics, with PC, OC4, and OC2 as dominant fractions of OC and with clear dominance of EC3 and EC2 over other EC fractions. The results obtained as part of this work may be a valuable source of information about the actual status of the carbonaceous matter, which remains one of the least known components of atmospheric PM.

Development of an improved two-sphere integration technique for quantifying black carbon concentrations in the atmosphere and seasonal snow

Abstract. An improved two-sphere integration (TSI) technique has been developed to quantify black carbon (BC) concentrations in the atmosphere and seasonal snow. The major advantage of this system is that it combines two distinct integrated spheres to reduce the scattering effect due to light-absorbing particles and thus provides accurate determinations of total light absorption from BC collected on Nuclepore filters. The TSI technique can be calibrated using a series of 15 filter samples of standard fullerene soot. This technique quantifies the mass of BC by separating the spectrally resolved total light absorption into BC and non-BC fractions. To assess the accuracy of the improved system, an empirical procedure for measuring BC concentrations with a two-step thermal–optical method is also applied. Laboratory results indicate that the BC concentrations determined using the TSI technique and theoretical calculations are well correlated (R2=0.99), whereas the thermal–optical method underestimates BC concentrations by 35 %–45 % compared to that measured by the TSI technique. Assessments of the two methods for atmospheric and snow samples revealed excellent agreement, with least-squares regression lines with slopes of 1.72 (r2=0.67) and 0.84 (r2=0.93), respectively. However, the TSI technique is more accurate in quantifications of BC concentrations in both the atmosphere and seasonal snow, with an overall lower uncertainty. Using the improved TSI technique, we find that light absorption at a wavelength of 550 nm due to BC plays a dominant role relative to non-BC light absorption in both the atmosphere (62.76 %–91.84 % of total light absorption) and seasonal snow (43.11 %–88.56 %) over northern China.

Quantification of elemental and total carbon in combustion particulate matter using thermal-oxidative analysis

ABSTRACT The use of a two-step thermal-oxidative analysis (TOA) technique for quantification of the mass of total carbon (TC) and elemental carbon (EC) of turbine engine-borne particulate matter (PM) has been evaluated. This approach could be used in lieu of analysis methods which were developed to characterize diluted PM. This effort is of particular interest as turbine engine PM emissions typically have a higher EC content than ambient aerosols, and filter sample mass loadings can be significantly greater than recommended for existing analysis techniques. Analyses were performed under a pure oxygen environment using a two-step temperature profile; reference carbon and actual PM samples were used to identify appropriate analysis conditions. Thermal gravimetric analysis (TGA) methods were used to provide guidance on the nature of the carbon in several of the materials. This was necessary as a standard reference material does not exist for determination of the EC fraction in PM. The TGA also assisted in identifying an appropriate temperature range for the first-stage of the TOA method. Quantification of TC and EC for turbine engine PM samples using TOA was compared to results obtained using the NIOSH 5040 thermal-optical method. For first-stage TOA temperatures of 350°C and 400°C, excellent agreement between the techniques was observed in both the quantified TC and EC, supporting the viability for using TOA for analysis of turbine engine PM samples. A primary benefit of using TOA for these types of PM samples is that filters with relatively high PM mass loadings (sampled at the emission source) can be readily analyzed. In addition, an entire filter sample can be evaluated, as compared to the use of a filter punch sample for the NIOSH technique. While the feasibility of using a TOA method for engine PM samples has been demonstrated, future studies to estimate potential OC charring and oxidation of EC-type material may provide additional data to assess its impact on the OC/EC fractions for other carbon-type measurements. Implications: This work presents results and procedures of an analytical method for the determination of total and elemental carbon, i.e., TC and EC present in combustion source particulate matter samples. In general, it is shown that the LECO TOA methodology is as reliable and comprehensive as NIOSH 5040 for determining TC and EC carbon types in particulate matter present in turbine emission sources, and should be considered as an alternative. Principles of the methodology, differences, and corresponding agreement with the standard NIOSH 5040 method and TGA analysis are discussed.

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