An evaluation of mass absorption cross-section for optical carbon analysis on Teflon filter media

Black carbon (BC) or elemental carbon (EC) is a by-product of incomplete fuel combustion, and contributes adversely to human health, visibility, and climate impacts. Previous studies have examined nondestructive techniques for particle light attenuation measurements on Teflon® filters to estimate BC. The incorporation of an inline Magee Scientific OT21 transmissometer into the MTL AH-225 robotic weighing system provides the opportunity to perform optical transmission measurements on Teflon filters at the same time as the gravimetric mass measurement. In this study, we characterize the performance of the inline OT21, and apply it to determine the mass absorption cross-section (MAC) of PM_2.5 BC across the United States. We analyzed 5393 archived Teflon® filters from the Chemical Speciation Network (CSN) collected during 2010–2011 and determined MAC by comparing light attenuation on Teflon® filters to corresponding thermal EC on quartz-fiber filters. Results demonstrated the importance of the initial transmission (I₀) value used in light attenuation calculations. While light transmission varied greatly within filter lots, the average I₀ of filter blanks during the sampling period provided an estimate for archived filters. For newly collected samples, it is recommended that filter-specific I₀ measurements be made (i.e., same filter before sample collection). The estimated MAC ranged from 6.9 to 9.4 m²/g and varied by region and season across the United States, indicating that using a default value may lead to under- or overestimated BC concentrations. An analysis of the chemical composition of these samples indicated good correlation with EC for samples with higher EC content as a fraction of total PM_2.5 mass, while the presence of light-scattering species such as crustal elements impacted the correlation affecting the MAC estimate. Overall, the method is demonstrated to be a quick, cost-effective approach to estimate BC from archived and newly sampled Teflon® filters by combining both gravimetric and BC measurements.

Implications: Robotic optical analysis is a valid, cost-effective means to obtain a vast amount of BC data from archived and current routine filters. A tailored mass absorption cross-section by region and season is necessary for a more representative estimate of BC. Initial light transmission measurements play an important role due to the variability in blank filter transmission. Combining gravimetric mass and BC analysis on a single Teflon® filter reduces costs for monitoring agencies and maximizes data collection.     

Evaluation of thermal optical analysis method of elemental carbon for marine fuel exhaust

The awareness of black carbon (BC) as the second largest anthropogenic contributor in global warming and an ice melting enhancer has increased. Due to prospected increase in shipping especially in the Arctic reliability of BC emissions and their invented amounts from ships is gaining more attention. The International Maritime Organization (IMO) is actively working toward estimation of quantities and effects of BC especially in the Arctic. IMO has launched work toward constituting a definition for BC and agreeing appropriate methods for its determination from shipping emission sources. In our study we evaluated the suitability of elemental carbon (EC) analysis by a thermal-optical transmittance (TOT) method to marine exhausts and possible measures to overcome the analysis interferences related to the chemically complex emissions. The measures included drying with CaSO_4, evaporation at 40–180ºC, H₂O treatment, and variation of the sampling method (in-stack and diluted) and its parameters (e.g., dilution ratio, Dr). A reevaluation of the nominal organic carbon (OC)/EC split point was made. Measurement of residual carbon after solvent extraction (TC-C_SOF) was used as a reference, and later also filter smoke number (FSN) measurement, which is dealt with in a forthcoming paper by the authors. Exhaust sources used for collecting the particle sample were mainly four-stroke marine engines operated with variable loads and marine fuels ranging from light to heavy fuel oils (LFO and HFO) with a sulfur content range of <0.1–2.4% S. The results were found to be dependent on many factors, namely, sampling, preparation and analysis method, and fuel quality. It was found that the condensed H₂SO₄ + H₂O on the particulate matter (PM) filter had an effect on the measured EC content, and also promoted the formation of pyrolytic carbon (PyC) from OC, affecting the accuracy of EC determination. Thus, uncertainty remained regarding the EC results from HFO fuels.

Implications: The work supports one part of the decision making in black carbon (BC) determination methodology. If regulations regarding BC emissions from marine engines will be implemented in the future, a well-defined and at best unequivocal method of BC determination is required for coherent and comparable emission inventories and estimating BC effects. As the aerosol from marine emission sources may be very heterogeneous and low in BC, special attention to the effects of sampling conditions and sample pretreatments on the validity of the results was paid in developing the thermal-optical analysis methodology (TOT).     

Public health and components of particulate matter: The changing assessment of black carbon

In 2012, the WHO classified diesel emissions as carcinogenic, and its European branch suggested creating a public health standard for airborne black carbon (BC). In 2011, EU researchers found that life expectancy could be extended four to nine times by reducing a unit of BC, vs reducing a unit of PM_2.5. Only recently could such determinations be made. Steady improvements in research methodologies now enable such judgments.

In this Critical Review, we survey epidemiological and toxicological literature regarding carbonaceous combustion emissions, as research methodologies improved over time. Initially, we focus on studies of BC, diesel, and traffic emissions in the Western countries (where daily urban BC emissions are mainly from diesels). We examine effects of other carbonaceous emissions, e.g., residential burning of biomass and coal without controls, mainly in developing countries.

Throughout the 1990s, air pollution epidemiology studies rarely included species not routinely monitored. As additional PM_2.5. chemical species, including carbonaceous species, became more widely available after 1999, they were gradually included in epidemiological studies. Pollutant species concentrations which more accurately reflected subject exposure also improved models.

Natural “interventions” - reductions in emissions concurrent with fuel changes or increased combustion efficiency; introduction of ventilation in highway tunnels; implementation of electronic toll payment systems – demonstrated health benefits of reducing specific carbon emissions. Toxicology studies provided plausible biological mechanisms by which different PM species, e.g., carbonaceous species, may cause harm, aiding interpretation of epidemiological studies.

Our review finds that BC from various sources appears to be causally involved in all-cause, lung cancer, and cardiovascular mortality, morbidity, and perhaps adverse birth and nervous system effects. We recommend that the U.S. EPA rubric for judging possible causality of PM_2.5. mass concentrations, be used to assess which PM_2.5. species are most harmful to public health.

Implications: Black carbon (BC) and correlated co-emissions appear causally related with all-cause, cardiovascular, and lung cancer mortality, and perhaps with adverse birth outcomes and central nervous system effects. Such findings are recent, since widespread monitoring for BC is also recent. Helpful epidemiological advances (using many health relevant PM_2.5 species in models; using better measurements of subject exposure) have also occurred. “Natural intervention” studies also demonstrate harm from partly combusted carbonaceous emissions. Toxicology studies consistently find biological mechanisms explaining how such emissions can cause these adverse outcomes. A consistent mechanism for judging causality for different PM_2.5 species is suggested.

A list of acronyms will be found at the end of the article.     

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

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.     

Comparison of measurement methods for the characterization of the black carbon emissions from a T63 turboshaft engine burning conventional and Fischer-Tropsch fuels

Emission measurements of black carbon (BC) mass were conducted on a T63 turboshaft engine, operated at idle and cruise power with conventional and alternative fuels, using an Artium LII-300 laser-induced incandescence analyzer (LII) and AVL model 483 micro soot sensor (MSS) photoacoustic instrument using the manufacturer’s calibration for both instruments. These measurements were compared with elemental carbon (EC) determined by manual and semicontinuous thermal-optical transmission analyses according to National Institute for Occupational Safety and Health (NIOSH) method 5040 as the reference method. The results indicate that both the LII and MSS instruments show good linear correlation with EC for the two fuels and two engine power conditions evaluated. The LII measurements were observed to be biased high (27–49%) and the MSS measurements were biased low (24–35%) relative to EC. The agreement between the instruments and the reference method was substantially improved by applying a calibration of the instruments against a common BC aerosol source. Test data also suggest that the two instruments show some sensitivity to particle size (or properties related to size), specifically for particles with a geometric mean diameter (GMD) <30 nm. This sensitivity is problematic, since new engines or certain combustion conditions in current engines will produce smaller particles compared with the T63 model tested in this study. Further assessments of instrument performance for particles within this size range are therefore warranted.

Implications: Accurate black carbon emission measurements are needed to certify new and in-production commercial aircraft engines. Both the Artium LII-300 and AVL 483 micro soot sensor are currently approved by the International Civil Aviation Organization for this purpose. This study compares the two instruments against elemental carbon (EC) using NIOSH method 5040 as the reference using a T63 turboshaft engine. The results indicate that both instruments correlate reasonably well with EC, and the correlation substantially improved when applying a calibration against a common aerosol source. Sensitivity to particle size may be an issue for both instruments.     

Comparison of the physical and chemical characteristics of fine road dust at different urban sites

The size distribution and chemical components of a fine fraction (<2.5 μm) of road dust collected at urban sites in Korea (Gwangju) and Mongolia (Ulaanbaatar) where distinct urban characteristics exist were measured. A clear bimodal size distribution was observed for the resuspended fine road dust at the urban sites in Korea. The first mode peaked at 100–110 nm, and the second peak was observed at 435–570 nm. Ultrafine mode (~30 nm) was found for the fine road dust at the Mongolia site, which was significantly affected by residential coal/biomass burning. The contribution of the water-soluble ions to the fine road dust was higher at the sites in Mongolia (15.8–16.8%) than at those in Korea (1.2–4.8%). Sulfate and chloride were the most dominant ionic species for the fine road dust in Mongolia. As (arsenic) was also much higher for the Mongolian road dust than the others. The sulfate, chloride, and As mainly come from coal burning activity, suggesting that coal and biomass combustion in Mongolia during the heating season should affect the size and chemical components of the fine road dust. Cu (copper) and Zn (zinc), carbonaceous particles (organic carbon [OC] and elemental carbon [EC]) increased at sites in Korea, suggesting that the fine road dust at these sites was significantly affected by the high volume of traffic (engine emission and brake/tire wear). Our results suggest that chemical profiles for road dust specific to certain sites should be applied to more accurately apportion road dust source contributing to the ambient particulate matter.

Implications: Size and chemical characteristics of fine road dust at sites having distinct urban characteristics were examined. Residential coal and biomass burning and traffic affected physiochemical properties of the fine road dust. Different road dust profiles at different sites should be needed to determine the ambient PM2.5 sources more accurately.     

The study on biomass fraction estimate methodology of municipal solid waste incinerator in Korea

In Korea, the amount of greenhouse gases released due to waste materials was 14,800,000 t CO₂eq in 2012, which increased from 5,000,000 t CO₂eq in 2010. This included the amount released due to incineration, which has gradually increased since 2010. Incineration was found to be the biggest contributor to greenhouse gases, with 7,400,000 t CO₂eq released in 2012. Therefore, with regards to the trading of greenhouse gases emissions initiated in 2015 and the writing of the national inventory report, it is important to increase the reliability of the measurements related to the incineration of waste materials.

This research explored methods for estimating the biomass fraction at Korean MSW incinerator facilities and compared the biomass fractions obtained with the different biomass fraction estimation methods. The biomass fraction was estimated by the method using default values of fossil carbon fraction suggested by IPCC, the method using the solid waste composition, and the method using incinerator flue gas.

The highest biomass fractions in Korean municipal solid waste incinerator facilities were estimated by the IPCC Default method, followed by the MSW analysis method and the Flue gas analysis method. Therefore, the difference in the biomass fraction estimate was the greatest between the IPCC Default and the Flue gas analysis methods. The difference between the MSW analysis and the flue gas analysis methods was smaller than the difference with IPCC Default method. This suggested that the use of the IPCC default method cannot reflect the characteristics of Korean waste incinerator facilities and Korean MSW.

Implications: Incineration is one of most effective methods for disposal of municipal solid waste (MSW). This paper investigates the applicability of using biomass content to estimate the amount of CO₂ released, and compares the biomass contents determined by different methods in order to establish a method for estimating biomass in the MSW incinerator facilities of Korea. After analyzing the biomass contents of the collected solid waste samples and the flue gas samples, the results were compared with the Intergovernmental Panel on Climate Change (IPCC) method, and it seems that to calculate the biomass fraction it is better to use the flue gas analysis method than the IPCC method. It is valuable to design and operate a real new incineration power plant, especially for the estimation of greenhouse gas emissions.     

Evaluation of the IMPROVE Equation for estimating aerosol light extinction

The [revised] IMPROVE Equation for estimating light extinction from aerosol chemical composition was evaluated considering new measurements at U.S. national parks. Compared with light scattering (Bsp) measured at seven IMPROVE sites with nephelometer data from 2003–2012, the [revised] IMPROVE Equation over- and underestimated Bsp in the lower and upper quintiles, respectively, of measured Bsp. Underestimation of the worst visibility cases (upper quintile) was reduced by assuming an organic mass (OM)/organic carbon (OC) ratio of 2.1 and hygroscopic growth of OM, based on results from previous field studies. This assumption, however, tended to overestimate low Bsp even more. Assuming that sulfate was present as ammonium bisulfate rather than as ammonium sulfate uniformly reduced estimated Bsp. The split-mode model of concentration- and size-dependent dry mass scattering efficiencies in the [revised] IMPROVE Equation does not eliminate systematic biases in estimated Bsp. While the new measurements of OM/OC and OM hygroscopicity should be incorporated into future iterations of the IMPROVE Equation, the problem is not well constrained due to a lack of routine measurements of sulfate neutralization and the water-soluble fraction of OM in the IMPROVE network.

Implications: Studies in U.S. national parks showed that aerosol organics contain more mass and absorb more water as a function of relative humidity than is currently assumed by the IMPROVE Equation for calculating chemical light extinction. Consideration of these results could significantly shift the apportionment of light extinction to water-soluble organic aerosols and therefore better inform pollution control strategies under the U.S. Environmental Protection Agency Regional Haze Rule.     

Influence of biowaste compost amendment on soil organic carbon storage under arid climate

Organic matter amendments have been proposed as a means to enhance soil carbon stocks on degraded soils, particularly under arid climate. Soil organic carbon (SOC) plays a critical role in terrestrial carbon cycling and is central to preserving soil quality. The effects of biowaste compost (BWC) on soil carbon storage were investigated. In addition, changes in soil organic matter (SOM) and even soil organic carbon (SOC) in BWC-amended soils following different applications were studied. The added BWC quantities were as followed: BWC/soil (weight/weight (w/w) respectively: 1/8, 1/4, and 1/2). The different BWC-amended soils were assessed during 180 days under arid ambient conditions and in comparison with control soil. Results showed a significant increase in SOM and SOC with relation to BWC quantities applied. This increase was relatively clear up to 120 days, after which decrease in SOM and SOC levels were observed. Furthermore, results showed improved microbiological activities of the amended soils in comparison with the control soil. This was reflected by the increase of the amended soils’ respirometric activities as cumulative carbon dioxide carbon (C-CO₂) as function of incubation time and also in terms of specific respiration expressed as C-CO₂/SOC ratios.

Implications: Mediterranean soils under arid climate such as Tunisian soils are poor in organic matter content. Biowastes are potential source for soil fertilization. Composting process is the best method for the stabilization of organic matter of diverse origins. The biowaste compost amendment improves the soil organic carbon storage and enhances the soil microbial activity.     

Real-time black carbon personal exposure levels in microenvironments: Home to home on a round-trip,Hanoi–Singapore

Little is known about personal exposure levels of black carbon (BC), a fraction of PM2.5, specifically in the transport microenvironments. In this study, real-time personal exposure to BC recorded by a portable microAeth AE51 was investigated in microenvironments in a round-trip from Hanoi (Vietnam) directly to Singapore. Personal exposure to BC was monitored in microenvironments at residential flat, in various surface modes of transport (taxi, bus, train), at the airports, and on the airplanes. The study found that personal exposure levels of BC in Singapore were higher than those in Hanoi for the same type of microenvironment in general for most of the microenvironments, except for smoking rooms. The highest exposures in each city were in smoking room in Noi Bai International Airport (NIA) and at bus station in Singapore, reached 98,709 ng/m3 and 44,513 ng/m3, respectively; the lowest personal exposure level was in-flight (approximately 250 ng/m3) for both trips. It is also remarkable that personal exposure to BC in indoor microenvironments was higher than outdoor levels.

Implications: Real-time personal exposure to BC was investigated in microenvironments in a round trip from Hanoi (Vietnam) directly to Singapore. BC personal exposure levels in Singapore were higher than those in Hanoi for the same type of microenvironment except for smoking rooms. Personal exposure to BC levels in indoor microenvironments was higher than in outdoor microenvironments. The highest levels of exposure were 98,709 ng/m3 in the smoking room at Noi Bai International Airport (Hanoi) and 44,513 ng/m3 at the bus station in Changi (Singapore). The lowest BC level was in-flight for both trips, at approximately 250 ng/m3.     

Carbonaceous aerosol emissions from India

Budget estimate for carbonaceous aerosols including black carbon (BC) and organic carbon, emitted from the combustion of various fuels, is very important for regional climate studies. Emission factors for carbonaceous aerosols from bio-fuels and soft coke were determined in a controlled combustion study. The emission factors thus obtained along with those available for other fossil fuels consumed in different sectors have been applied to assess the budget for carbonaceous aerosols from India. Preliminary calculations give a range of 1.6–1.8 Tg of carbonaceous aerosols that include 0.4–1.4 Tg of BC. A major (80%) portion of carbonaceous aerosols emitted from India is found to originate from the use of biomass for energy as 70–80% of energy requirement in rural India is met by combustion of traditional bio-fuels.     

Emission factors of fine particulate matter,organic and elemental carbon,carbon monoxide,and carbon dioxide for four solid fuels commonly used in residential heating by the U.S. Navajo Nation

Most homes in the Navajo Nation use wood as their primary heating fuel, often in combination with locally mined coal. Previous studies observed health effects linked to this solid-fuel use in several Navajo communities. Emission factors (EFs) for common fuels used by the Navajo have not been reported using a relevant stove type. In this study, two softwoods (ponderosa pine and Utah juniper) and two high-volatile bituminous coals (Black Mesa and Fruitland) were tested with an in-use residential conventional wood stove (homestove) using a modified American Society for Testing and Materials/U.S. Environmental Protection Agency (ASTM/EPA) protocol. Filter sampling quantified PM_2.5 (particulate matter with an aerodynamic diameter ≤2.5 μm) and organic (OC) and elemental (EC) carbon in the emissions. Real-time monitoring quantified carbon monoxide (CO), carbon dioxide (CO₂), and total suspended particles (TSP). EFs for these air pollutants were developed and normalized to both fuel mass and energy consumed. In general, coal had significantly higher mass EFs than wood for all pollutants studied. In particular, coal emitted, on average, 10 times more PM_2.5 than wood on a mass basis, and 2.4 times more on an energy basis. The EFs developed here were based on fuel types, stove design, and operating protocols relevant to the Navajo Nation, but they could be useful to other Native Nations with similar practices, such as the nearby Hopi Nation.

Implications: Indoor wood and coal combustion is an important contributor to public health burdens in the Navajo Nation. Currently, there exist no emission factors representative of Navajo homestoves, fuels, and practices. This study developed emission factors for PM_2.5, OC, EC, CO, and CO₂ using a representative Navajo homestove. These emission factors may be utilized in regional-, national-, and global-scale health and environmental models. Additionally, the protocols developed and results presented here may inform on-going stove design of the first EPA-certified wood and coal combination stove.     

Impacts of prescribed fires and benefits from their reduction for air quality,health, and visibility in the Pacific Northwest of the United States

Using a WRF-SMOKE-CMAQ modeling framework, we investigate the impacts of smoke from prescribed fires on model performance, regional and loc al air quality, health impacts, and visibility in protected natural environments using three different prescribed fire emission scenarios: 100% fire, no fire, and 30% fire. The 30% fire case reflects a 70% reduction in fire activities due to harvesting of logging residues for use as a feedstock for a potential aviation biofuel supply chain. Overall model performance improves for several performance metrics when fire emissions are included, especially for organic carbon, irrespective of the model goals and criteria used. This effect on model performance is more pronounced for the rural and remote IMPROVE sites for organic carbon and total PM_2.5. A reduction in prescribed fire emissions (30% fire case) results in significant improvement in air quality in areas in western Oregon, northern Idaho, and western Montana, where most prescribed fires occur. Prescribed burning contributes to visibility impairment, and a relatively large portion of protected class I areas will benefit from a reduced emission scenario. For the haziest 20% days, prescribed burning is an important source of visibility impairment, and approximately 50% of IMPROVE sites in the model domain show a significant improvement in visibility for the reduced fire case. Using BenMAP, a health impact assessment tool, we show that several hundred additional deaths, several thousand upper and lower respiratory symptom cases, several hundred bronchitis cases, and more than 35,000 workday losses can be attributed to prescribed fires, and these health impacts decrease by 25–30% when a 30% fire emission scenario is considered.

Implications: This study assesses the potential regional and local air quality, public health, and visibility impacts from prescribed burning activities, as well as benefits that can be achieved by a potential reduction in emissions for a scenario where biomass is harvested for conversion to biofuel. As prescribed burning activities become more frequent, they can be more detrimental for air quality and health. Forest residue-based biofuel industry can be source of cleaner fuel with co-benefits of improved air quality, reduction in health impacts, and improved visibility.     

Evaluation of solid particle number and black carbon for very low particulate matter emissions standards in light-duty vehicles

To reliably measure at the low particulate matter (PM) levels needed to meet California’s Low Emission Vehicle (LEV III) 3- and 1-mg/mile particulate matter (PM) standards, various approaches other than gravimetric measurement have been suggested for testing purposes. In this work, a feasibility study of solid particle number (SPN, d50 = 23 nm) and black carbon (BC) as alternatives to gravimetric PM mass was conducted, based on the relationship of these two metrics to gravimetric PM mass, as well as the variability of each of these metrics. More than 150 Federal Test Procedure (FTP-75) or Supplemental Federal Test Procedure (US06) tests were conducted on 46 light-duty vehicles, including port-fuel-injected and direct-injected gasoline vehicles, as well as several light-duty diesel vehicles equipped with diesel particle filters (LDD/DPF). For FTP tests, emission variability of gravimetric PM mass was found to be slightly less than that of either SPN or BC, whereas the opposite was observed for US06 tests. Emission variability of PM mass for LDD/DPF was higher than that of both SPN and BC, primarily because of higher PM mass measurement uncertainties (background and precision) near or below 0.1 mg/mile. While strong correlations were observed from both SPN and BC to PM mass, the slopes are dependent on engine technologies and driving cycles, and the proportionality between the metrics can vary over the course of the test. Replacement of the LEV III PM mass emission standard with one other measurement metric may imperil the effectiveness of emission reduction, as a correlation-based relationship may evolve over future technologies for meeting stringent greenhouse standards.

Implications: Solid particle number and black carbon were suggested in place of PM mass for the California LEV III 1-mg/mile FTP standard. Their equivalence, proportionality, and emission variability in comparison to PM mass, based on a large light-duty vehicle fleet examined, are dependent on engine technologies and driving cycles. Such empirical derived correlations exhibit the limitation of using these metrics for enforcement and certification standards as vehicle combustion and after-treatment technologies advance.     

Particle count and black carbon measurements at schools in Las Vegas,NV and in the greater Salt Lake City,UT area

As part of two separate studies aimed to characterize ambient pollutant concentrations at schools in urban areas, we compare black carbon and particle count measurements at Adcock Elementary in Las Vegas, NV (April–June 2013), and Hunter High School in the West Valley City area of greater Salt Lake City, UT (February 2012). Both schools are in urban environments, but Adcock Elementary is next to the U.S. 95 freeway. Black carbon (BC) concentrations were 13% higher at Adcock compared to Hunter, while particle count concentrations were 60% higher. When wind speeds were low—less than 2 m/sec—both BC and particle count concentrations were significantly higher at Adcock, while concentrations at Hunter did not have as strong a variation with wind speed. When wind speeds were less than 2 m/sec, emissions from the adjacent freeway greatly affected concentrations at Adcock, regardless of wind direction. At both sites, BC and particle count concentrations peaked in the morning during commute hours. At Adcock, particle count also peaked during midday or early afternoon, when BC was low and conditions were conducive to new particle formation. While this midday peak occurred at Adcock on roughly 45% of the measured days, it occurred on only about 25% of the days at Hunter, since conditions for particle formation (higher solar radiation, lower wind speeds, lower relative humidity) were more conducive at Adcock. Thus, children attending these schools are likely to be exposed to pollution peaks during school drop-off in the morning, when BC and particle count concentrations peak, and often again during lunchtime recess when particle count peaks again.

Implications: Particle count concentrations at two schools were shown to typically be independent of BC or other pollutants. At a school in close proximity to a major freeway, particle count concentrations were high during the midday and when wind speeds were low, regardless of wind direction, showing a large area of effect from roadway emissions even when the school was not downwind of the roadway. At the second school, which sits in an urban neighborhood away from freeways, high particle counts occurred even though solar radiation was low during wintertime conditions, meaning that exposure to high particle counts can occur throughout the year.     

Urban impacts on regional carbonaceous aerosols: Case study in central Texas

Rural and background sites provide valuable information on the concentration and optical properties of organic, elemental, and water-soluble organic carbon (OC, EC, and WSOC), which are relevant for understanding the climate forcing potential of regional atmospheric aerosols. To quantify climate- and air quality-relevant characteristics of carbonaceous aerosol in the central United States, a regional background site in central Texas was chosen for long-term measurement. Back trajectory (BT) analysis, ambient OC, EC, and WSOC concentrations and absorption parameters are reported for the first 15 months of a long-term campaign (May 2011–August 2012). BT analysis indicates consistent north–south airflow connecting central Texas to the Central Plains. Central Texas aerosols exhibited seasonal trends with increased fine particulate matter (<2.5 μm aerodynamic diameter, PM_2.5) and OC during the summer (PM_2.5 = 10.9 μg m^?3 and OC = 3.0 μg m^?3) and elevated EC during the winter (0.22 μg m^?3). When compared to measurements in Dallas and Houston, TX, central Texas OC appears to have mixed urban and rural sources. However, central Texas EC appears to be dominated by transport of urban emissions. WSOC averaged 63% of the annual OC, with little seasonal variability in this ratio. To monitor brown carbon (BrC), absorption was measured for the aqueous WSOC extracts. Light absorption coefficients for EC and BrC were highest during summer (EC MAC = 11 m² g^?1 and BRC MAE₃₆₅ = 0.15 m² g^?1). Results from optical analysis indicate that regional aerosol absorption is mostly due to EC with summertime peaks in BrC attenuation. This study represents the first reported values of WSOC absorption, MAE₃₆₅, for the central United States.

Implications:Background concentration and absorption measurements are essential in determining regional potential radiative forcing due to atmospheric aerosols. Back trajectory, chemical, and optical analysis of PM_2.5 was used to determine climatic and air quality implications of urban outflow to a regional receptor site, representative of the central United States. Results indicate that central Texas organic carbon has mixed urban and rural sources, while elemental carbon is controlled by the transport of urban emissions. Analysis of aerosol absorption showed black carbon as the dominant absorber, with less brown carbon absorption than regional studies in California and the southeastern United States.     

Quantification and radiocarbon source apportionment of black carbon in atmospheric aerosols using the CTO-375 method

To make progress towards linking the atmosphere and biogeosphere parts of the black carbon (BC) cycle, a chemothermal oxidation method (CTO-375), commonly applied for isolating BC from complex geomatrices such as soils, sediments and aquatic particles, was applied to investigate the BC also in atmospheric particles. Concentrations and ¹⁴C-based source apportionment of CTO-375 based BC was established for a reference aerosol (NIST RM-8785) and for wintertime aerosols collected in Stockholm and in a Swedish background area. The results were compared with thermal–optical (OC/EC) measurements. For NIST RM-8785, a good agreement was found between the BC_CTO-375 concentration and the reported elemental carbon (EC) concentration measured by the “Speciation Trends Network—National Institute of Occupational Safety and Health” method (EC_NIOSH) with BC_CTO-375 of 0.054±0.002 g g⁻¹ and EC_NIOSH of 0.067±0.008 g g⁻¹. In contrast, there was an average factor of ca. 20 difference between BC_CTO-375 and EC_NIOSH for the ambient Scandinavian wintertime aerosols, presumably reflecting a combination of BC_CTO-375 isolating only the recalcitrant soot-BC portion of the BC continuum and the EC_NIOSH metric inadvertently including some intrinsically non-pyrogenic organic matter. Isolation of BC_CTO-375 with subsequent off-line radiocarbon analysis yielded fraction modern values (fM) for total organic carbon (TOC) of 0.93 (aerosols from a Swedish background area), and 0.58 (aerosols collected in Stockholm); whereas the fM for BC_CTO-375 isolates were 1.08 (aerosols from a Swedish background area), and 0.87 (aerosols collected in Stockholm). This radiocarbon-based source apportionment suggests that contribution from biomass combustion to cold-season atmospheric BC_CTO-375 in Stockholm was 70% and in the background area 88%.     

Hourly measurements of fine particulate sulfate and carbon aerosols at the Harvard-U.S. Environmental Protection Agency Supersite in Boston

Hourly concentrations of ambient fine particle sulfate and carbonaceous aerosols (elemental carbon [EC], organic carbon [OC], and black carbon [BC]) were measured at the Harvard-U.S. Environmental Protection Agency Supersite in Boston, MA, between January 2007 and October 2008. These hourly concentrations were compared with those made using integrated filter-based measurements over 6-day or 24-hr periods. For sulfate, the two measurement methods showed good agreement. Semicontinuous measurements of EC and OC also agreed (but not as well as for sulfate) with those obtained using 24-hr integrated filter-based and optical BC reference methods. During the study period, 24-hr PM2.5 (particulate matter [PM] < or = 2.5 microm in aerodynamic diameter) concentrations ranged from 1.4 to 37.6 microg/m3, with an average of 9.3 microg/m3. Sulfate as the equivalent of ammonium sulfate accounted for 39.1% of the PM2.5 mass, whereas EC and OC accounted for 4.2 and 35.2%, respectively. Hourly sulfate concentrations showed no distinct diurnal pattern, whereas hourly EC and BC concentrations peaked during the morning rush hour between 7:00 and 9:00 a.m. OC concentrations also exhibited nonpronounced, small peaks during the day, most likely related to traffic, secondary organic aerosol, and local sources, respectively.     

Synthesis of Harvard Environmental Protection Agency (EPA) Center studies on traffic-related particulate pollution and cardiovascular outcomes in the Greater Boston Area

The association between particulate pollution and cardiovascular morbidity and mortality is well established. While the cardiovascular effects of nationally regulated criteria pollutants (e.g., fine particulate matter [PM_2.5] and nitrogen dioxide) have been well documented, there are fewer studies on particulate pollutants that are more specific for traffic, such as black carbon (BC) and particle number (PN). In this paper, we synthesized studies conducted in the Greater Boston Area on cardiovascular health effects of traffic exposure, specifically defined by BC or PN exposure or proximity to major roadways. Large cohort studies demonstrate that exposure to traffic-related particles adversely affect cardiac autonomic function, increase systemic cytokine-mediated inflammation and pro-thrombotic activity, and elevate the risk of hypertension and ischemic stroke. Key patterns emerged when directly comparing studies with overlapping exposure metrics and population cohorts. Most notably, cardiovascular risk estimates of PN and BC exposures were larger in magnitude or more often statistically significant compared to those of PM_2.5 exposures. Across multiple exposure metrics (e.g., short-term vs. long-term; observed vs. modeled) and different population cohorts (e.g., elderly, individuals with co-morbidities, young healthy individuals), there is compelling evidence that BC and PN represent traffic-related particles that are especially harmful to cardiovascular health. Further research is needed to validate these findings in other geographic locations, characterize exposure errors associated with using monitored and modeled traffic pollutant levels, and elucidate pathophysiological mechanisms underlying the cardiovascular effects of traffic-related particulate pollutants.

Implications: Traffic emissions are an important source of particles harmful to cardiovascular health. Traffic-related particles, specifically BC and PN, adversely affect cardiac autonomic function, increase systemic inflammation and thrombotic activity, elevate BP, and increase the risk of ischemic stroke. There is evidence that BC and PN are associated with greater cardiovascular risk compared to PM_2.5. Further research is needed to elucidate other health effects of traffic-related particles and assess the feasibility of regulating BC and PN or their regional and local sources.     

BTEX exposures in an area impacted by industrial and mobile sources: Source attribution and impact of averaging time

The impacts of emissions plumes from major industrial sources on black carbon (BC) and BTEX (benzene, toluene, ethyl benzene, xylene isomers) exposures in communities located >10 km from the industrial source areas were identified with a combination of stationary measurements, source identification using positive matrix factorization (PMF), and dispersion modeling. The industrial emissions create multihour plume events of BC and BTEX at the measurement sites. PMF source apportionment, along with wind patterns, indicates that the observed pollutant plumes are the result of transport of industrial emissions under conditions of low boundary layer height. PMF indicates that industrial emissions contribute >50% of outdoor exposures of BC and BTEX species at the receptor sites. Dispersion modeling of BTEX emissions from known industrial sources predicts numerous overnight plumes and overall qualitative agreement with PMF analysis, but predicts industrial impacts at the measurement sites a factor of 10 lower than PMF. Nonetheless, exposures associated with pollutant plumes occur mostly at night, when residents are expected to be home but are perhaps unaware of the elevated exposure. Averaging data samples over long times typical of public health interventions (e.g., weekly or biweekly passive sampling) misapportions the exposure, reducing the impact of industrial plumes at the expense of traffic emissions, because the longer samples cannot resolve subdaily plumes. Suggestions are made for ways for future distributed pollutant mapping or intervention studies to incorporate high time resolution tools to better understand the potential impacts of industrial plumes.

Implications: Emissions from industrial or other stationary sources can dominate air toxics exposures in communities both near the source and in downwind areas in the form of multihour plume events. Common measurement strategies that use highly aggregated samples, such as weekly or biweekly averages, are insensitive to such plume events and can lead to significant under apportionment of exposures from these sources.