Primary Carbonaceous Aerosols Research Articles

Toxicological Effects of Secondary Air Pollutants.

Secondary air pollutants, originating from gaseous pollutants and primary particulate matter emitted by natural sources and human activities, undergo complex atmospheric chemical reactions and multiphase processes. Secondary gaseous pollutants represented by ozone and secondary particulate matter, including sulfates, nitrates, ammonium salts, and secondary organic aerosols, are formed in the atmosphere, affecting air quality and human health. This paper summarizes the formation pathways and mechanisms of important atmospheric secondary pollutants. Meanwhile, different secondary pollutants' toxicological effects and corresponding health risks are evaluated. Studies have shown that secondary pollutants are generally more toxic than primary ones. However, due to their diverse source and complex generation mechanism, the study of the toxicological effects of secondary pollutants is still in its early stages. Therefore, this paper first introduces the formation mechanism of secondary gaseous pollutants and focuses mainly on ozone's toxicological effects. In terms of particulate matter, secondary inorganic and organic particulate matters are summarized separately, then the contribution and toxicological effects of secondary components formed from primary carbonaceous aerosols are discussed. Finally, secondary pollutants generated in the indoor environment are briefly introduced. Overall, a comprehensive review of secondary air pollutants may shed light on the future toxicological and health effects research of secondary air pollutants.

Fire Aerosols Slow Down the Global Water Cycle

Abstract Fire is an important Earth system process and the largest source of global primary carbonaceous aerosols. Earlier studies have focused on the influence of fire aerosols on radiation, surface climate, air quality, and biogeochemical cycle. The impact of fire aerosols on the global water cycle has not been quantified and related mechanisms remain largely unclear. This study provides the first quantitative assessment and understanding of the influence of fire aerosols on the global water cycle. This is done by quantifying the difference between simulations with and without fire aerosols using the coupled Community Earth System Model (CESM). Results show that present-day fire aerosols weaken the global water cycle significantly. They decrease the continental precipitation, evapotranspiration, and runoff by 4.1 ± 1.8, 2.5 ± 0.5, and 1.5 ± 1.4 ×103 km3 yr−1 as well as ocean evaporation, precipitation, and water vapor transport from ocean to land by 8.1 ± 1.9, 6.6 ± 2.3, and 1.5 ± 1.4 ×103 km3 yr−1. The impacts of fire aerosols are most clearly seen in the tropics and the Arctic-boreal zone. Fire aerosols affect the global water cycle mainly by cooling the surface, which reduces ocean evaporation, land soil evaporation, and plant transpiration. The decreased water vapor load in the atmosphere leads to a decrease in precipitation, which contributes to reduced surface runoff and subsurface drainage.

Elucidating the present-day chemical composition, seasonality and source regions of climate-relevant aerosols across the Arctic land surface

The Arctic is warming two to three times faster than the global average, and the role of aerosols is not well constrained. Aerosol number concentrations can be very low in remote environments, rendering local cloud radiative properties highly sensitive to available aerosol. The composition and sources of the climate-relevant aerosols, affecting Arctic cloud formation and altering their microphysics, remain largely elusive due to a lack of harmonized concurrent multi-component, multi-site, and multi-season observations. Here, we present a dataset on the overall chemical composition and seasonal variability of the Arctic total particulate matter (with a size cut at 10 μm, PM10, or without any size cut) at eight observatories representing all Arctic sectors. Our holistic observational approach includes the Russian Arctic, a significant emission source area with less dedicated aerosol monitoring, and extends beyond the more traditionally studied summer period and black carbon/sulfate or fine-mode pollutants. The major airborne Arctic PM components in terms of dry mass are sea salt, secondary (non-sea-salt, nss) sulfate, and organic aerosol (OA), with minor contributions from elemental carbon (EC) and ammonium. We observe substantial spatiotemporal variability in component ratios, such as EC/OA, ammonium/nss-sulfate and OA/nss-sulfate, and fractional contributions to PM. When combined with component-specific back-trajectory analysis to identify marine or terrestrial origins, as well as the companion study by Moschos et al 2022 Nat. Geosci. focusing on OA, the composition analysis provides policy-guiding observational insights into sector-based differences in natural and anthropogenic Arctic aerosol sources. In this regard, we first reveal major source regions of inner-Arctic sea salt, biogenic sulfate, and natural organics, and highlight an underappreciated wintertime source of primary carbonaceous aerosols (EC and OA) in West Siberia, potentially associated with the oil and gas sector. The presented dataset can assist in reducing uncertainties in modelling pan-Arctic aerosol-climate interactions, as the major contributors to yearly aerosol mass can be constrained. These models can then be used to predict the future evolution of individual inner-Arctic atmospheric PM components in light of current and emerging pollution mitigation measures and improved region-specific emission inventories.

Characteristics and source origins of carbonaceous aerosol in fine particulate matter in a megacity, Sichuan Basin, southwestern China

This paper reports the temporal variations, sources and transport characteristics of carbonaceous aerosol in Chongqing, a megacity in the Sichuan Basin. Hourly organic carbon (OC) and elemental carbon (EC) mass concentrations in PM2.5 were measured at an urban supersite from November 2019 to October 2020. The annual mean PM2.5, OC and EC concentrations (±1SD) were 38.50 ± 25.79 μg/m3, 9.03 ± 5.73 and 2.45 ± 1.47 μgC/m3, respectively. An intensive influence of biomass combustion was found during the observation period. Strong seasonality of carbonaceous aerosol with highest concentrations in winter and lowest concentrations in summer was observed. Meanwhile, two diverse pathways for secondary formation dominated in different seasons. One was highly related to gas-phase photochemical oxidation under high temperature and radiation, and another was highly related to heterogeneous reactions, while the latter was more significant, especially in winter. Diurnal and quarterly variation patterns for carbonaceous aerosol showed that the development of planetary boundary layer strongly influenced carbonaceous aerosol concentrations. Moreover, the regional sources from the northeast within the basin were identified as major contributors of the primary carbonaceous aerosol to Chongqing, while secondary components were more from local sources than regional transport. This study highlights the importance of prioritising the abatement of gaseous precursors for carbonaceous aerosol and an urgent need for the inter-regional prevention and control measures of the cities located in the Sichuan basin, especially the cities in the northeast of urban Chongqing.

Characteristics of fine carbonaceous aerosols in Wuhai, a resource-based city in Northern China:Insights from energy efficiency and population density

As one of the predominant compositions of PM2.5 (particulate matter with aerodynamic diameter ≤2.5 μm), carbonaceous aerosols not only have adverse effects on air quality, but also can affect climate change. Although there are extensive recent studies on carbonaceous aerosols, comprehensive studies on their socioeconomic influencing factors in a resource-based city are relatively limited. In this study, the spatial-temporal variations of organic carbon (OC), elemental carbon (EC), and secondary organic carbon (SOC) were investigated in January, July, and October in 2015 and April in 2016 in Wuhai and its surrounding areas. The population distribution and industry layout have led to the uneven spatial-temporal distribution of carbonaceous aerosols. The concentrations of carbonaceous aerosols were higher in winter due to the unfavorable meteorology and the increased emissions from heating. The SOC is a significant contributor to OC in the cold season (52.0% for January). Primary carbonaceous aerosols pollution is higher in the industrial sites of resource-based cities, whereas the SOC makes a significant contribution in the residential sites. The results of backward-trajectory and concentration-weighted trajectory analysis suggest that the local emissions and short-range atmospheric transport from nearby areas have a significant impact on PM2.5 and carbonaceous aerosols. A strong correlation between population density and OC/EC ratio was found, indicating that the megacities with high population density have a higher SOC contribution than the resource-based cities. Resource-based cities are characterized by high level of primary OC emissions, whereas cities with high energy efficiency have a more significant SOC contribution. These results provide a more comprehensive understanding of carbonaceous aerosols in a resource-based city.

Seasonal variation and size distributions of water-soluble inorganic ions and carbonaceous aerosols at a coastal site in Ningbo, China

Size-fractioned aerosol samples were collected by an eight-stage Anderson sampler for four seasons from November 2014 to August 2015 at a coastal and suburban site in Ningbo, China, with a total of 270 samples were obtained. The seasonal variations and size distributions of water-soluble inorganic ions (WSIIs), carbonaceous aerosols (OC and EC), which consist of four organic carbon (OC1-OC4), pyrolyzed carbon (OP) and three elemental carbon fraction (EC1-EC3), were investigated. For the sampling periods, the average total concentration of WSIIs, OC and EC in PM1.1, PM1.1–2.1 and PM2.1–9.0 were 21.3 ± 7 μg/m3, 6.7 ± 2.7 μg/m3 and 12.8 ± 1.9 μg/m3, constituting 75.5%, 62.7% and 43.2% of the different size particle mass, respectively. The predominant chemical species were SO42−, NO3−, and OC. WSIIs, OC and EC all exhibited significant difference between PM2.1 and PM2.1–9.0, reflecting their different sources. Ion balance calculations showed that the acidity of aerosols increased with a decrease in size, with the maximum of 1.07 in 1.1–2.1 μm and the minimum of 0.47 in 2.1–9 μm. It showed that size distributions of high-temperature carbon fraction such as OC4, OP and EC1 were almost unimodal during all seasons as well as SO42− and NH4+, in contrast, that of lower temperature carbon fraction (OC1-OC3), Mg2+, and Ca2+ appear like bimodal. Furthermore, the high consistency between the size distribution of OC4, OP and SO42−, NH4+ in all seasons suggests that the similar or related generation process for the secondary organic and inorganic/ionic species, which contribute the most significant component of the particulate matter. Besides the secondary aerosols, primary carbonaceous aerosols (PC), which may originate in emissions from mixed combustion or natural source, also contributed a significant fraction of haze pollution, especially in autumn, spring and summer.

Global anthropogenic emissions of particulate matter including black carbon

Abstract. This paper presents a comprehensive assessment of historical (1990–2010) global anthropogenic particulate matter (PM) emissions including the consistent and harmonized calculation of mass-based size distribution (PM1, PM2. 5, PM10), as well as primary carbonaceous aerosols including black carbon (BC) and organic carbon (OC). The estimates were developed with the integrated assessment model GAINS, where source- and region-specific technology characteristics are explicitly included. This assessment includes a number of previously unaccounted or often misallocated emission sources, i.e. kerosene lamps, gas flaring, diesel generators, refuse burning; some of them were reported in the past for selected regions or in the context of a particular pollutant or sector but not included as part of a total estimate. Spatially, emissions were calculated for 172 source regions (as well as international shipping), presented for 25 global regions, and allocated to 0.5° × 0.5° longitude–latitude grids. No independent estimates of emissions from forest fires and savannah burning are provided and neither windblown dust nor unpaved roads emissions are included. We estimate that global emissions of PM have not changed significantly between 1990 and 2010, showing a strong decoupling from the global increase in energy consumption and, consequently, CO2 emissions, but there are significantly different regional trends, with a particularly strong increase in East Asia and Africa and a strong decline in Europe, North America, and the Pacific region. This in turn resulted in important changes in the spatial pattern of PM burden, e.g. European, North American, and Pacific contributions to global emissions dropped from nearly 30 % in 1990 to well below 15 % in 2010, while Asia's contribution grew from just over 50 % to nearly two-thirds of the global total in 2010. For all PM species considered, Asian sources represented over 60 % of the global anthropogenic total, and residential combustion was the most important sector, contributing about 60 % for BC and OC, 45 % for PM2. 5, and less than 40 % for PM10, where large combustion sources and industrial processes are equally important. Global anthropogenic emissions of BC were estimated at about 6.6 and 7.2 Tg in 2000 and 2010, respectively, and represent about 15 % of PM2. 5 but for some sources reach nearly 50 %, i.e. for the transport sector. Our global BC numbers are higher than previously published owing primarily to the inclusion of new sources. This PM estimate fills the gap in emission data and emission source characterization required in air quality and climate modelling studies and health impact assessments at a regional and global level, as it includes both carbonaceous and non-carbonaceous constituents of primary particulate matter emissions. The developed emission dataset has been used in several regional and global atmospheric transport and climate model simulations within the ECLIPSE (Evaluating the Climate and Air Quality Impacts of Short-Lived Pollutants) project and beyond, serves better parameterization of the global integrated assessment models with respect to representation of black carbon and organic carbon emissions, and built a basis for recently published global particulate number estimates.

Description and evaluation of a new four-mode version of the Modal Aerosol Module (MAM4) within version 5.3 of the Community Atmosphere Model

Abstract. Atmospheric carbonaceous aerosols play an important role in the climate system by influencing the Earth's radiation budgets and modifying the cloud properties. Despite the importance, their representations in large-scale atmospheric models are still crude, which can influence model simulated burden, lifetime, physical, chemical and optical properties, and the climate forcing of carbonaceous aerosols. In this study, we improve the current three-mode version of the Modal Aerosol Module (MAM3) in the Community Atmosphere Model version 5 (CAM5) by introducing an additional primary carbon mode to explicitly account for the microphysical ageing of primary carbonaceous aerosols in the atmosphere. Compared to MAM3, the four-mode version of MAM (MAM4) significantly increases the column burdens of primary particulate organic matter (POM) and black carbon (BC) by up to 40 % in many remote regions, where in-cloud scavenging plays an important role in determining the aerosol concentrations. Differences in the column burdens for other types of aerosol (e.g., sulfate, secondary organic aerosols, mineral dust, sea salt) are less than 1 %. Evaluating the MAM4 simulation against in situ surface and aircraft observations, we find that MAM4 significantly improves the simulation of seasonal variation of near-surface BC concentrations in the polar regions, by increasing the BC concentrations in all seasons and particularly in cold seasons. However, it exacerbates the overestimation of modeled BC concentrations in the upper troposphere in the Pacific regions. The comparisons suggest that, to address the remaining model POM and BC biases, future improvements are required related to (1) in-cloud scavenging and vertical transport in convective clouds and (2) emissions of anthropogenic and biomass burning aerosols.

Global climate impacts of country-level primary carbonaceous aerosol from solid-fuel cookstove emissions

Cookstove use is globally one of the largest unregulated anthropogenic sources of primary carbonaceous aerosol. While reducing cookstove emissions through national-scale mitigation efforts has clear benefits for improving indoor and ambient air quality, and significant climate benefits from reduced green-house gas emissions, climate impacts associated with reductions to co-emitted black (BC) and organic carbonaceous aerosol are not well characterized. Here we attribute direct, indirect, semi-direct, and snow/ice albedo radiative forcing (RF) and associated global surface temperature changes to national-scale carbonaceous aerosol cookstove emissions. These results are made possible through the use of adjoint sensitivity modeling to relate direct RF and BC deposition to emissions. Semi- and indirect effects are included via global scaling factors, and bounds on these estimates are drawn from current literature ranges for aerosol RF along with a range of solid fuel emissions characterizations. Absolute regional temperature potentials are used to estimate global surface temperature changes. Bounds are placed on these estimates, drawing from current literature ranges for aerosol RF along with a range of solid fuel emissions characterizations. We estimate a range of 0.16 K warming to 0.28 K cooling with a central estimate of 0.06 K cooling from the removal of cookstove aerosol emissions. At the national emissions scale, countries’ impacts on global climate range from net warming (e.g., Mexico and Brazil) to net cooling, although the range of estimated impacts for all countries span zero given uncertainties in RF estimates and fuel characterization. We identify similarities and differences in the sets of countries with the highest emissions and largest cookstove temperature impacts (China, India, Nigeria, Pakistan, Bangladesh and Nepal), those with the largest temperature impact per carbon emitted (Kazakhstan, Estonia, and Mongolia), and those that would provide the most efficient cooling from a switch to fuel with a lower BC emission factor (Kazakhstan, Estonia, and Latvia). The results presented here thus provide valuable information for climate impact assessments across a wide range of cookstove initiatives.

Patterns in atmospheric carbonaceous aerosols in China: emission estimates and observed concentrations

Abstract. China is experiencing severe carbonaceous aerosol pollution driven mainly by large emissions resulting from intensive use of solid fuels. To gain a better understanding of the levels and trends of carbonaceous aerosol emissions and the resulting ambient concentrations at the national scale, we update an emission inventory of anthropogenic organic carbon (OC) and elemental carbon (EC) and employ existing observational studies to analyze characteristics of these aerosols including temporal, spatial, and size distributions, and the levels and shares of secondary organic carbon (SOC) in total OC. We further use ground observations to test the levels and inter-annual trends of the calculated national and provincial emissions of carbonaceous aerosols, and propose possible improvements in emission estimation for the future. The national OC emissions are estimated to have increased 29 % from 2000 (2127 Gg) to 2012 (2749 Gg) and EC by 37 % (from 1356 to 1857 Gg). The residential, industrial, and transportation sectors contributed an estimated 74–78, 17–21, and 4–6 % of the total emissions of OC, respectively, and 49–55, 30–34, and 14–18 % of EC. Updated emission factors (EFs) based on the most recent local field measurements, particularly for biofuel stoves, led to considerably lower emissions of OC compared to previous inventories. Compiling observational data across the country, higher concentrations of OC and EC are found in northern and inland cities, while higher OC / EC ratios are found in southern sites, due to the joint effects of primary emissions and meteorology. Higher OC / EC ratios are estimated at rural and remote sites compared to urban ones, attributed to more emissions of OC from biofuel use, more biogenic emissions of volatile organic compound (VOC) precursors to SOC, and/or transport of aged aerosols. For most sites, higher concentrations of OC, EC, and SOC are observed in colder seasons, while SOC / OC is reduced, particularly at rural and remote sites, attributed partly to weaker atmospheric oxidation and SOC formation compared to summer. Enhanced SOC formation from oxidization and anthropogenic activities like biomass combustion is judged to have crucial effects on severe haze events characterized by high particle concentrations. Several observational studies indicate an increasing trend in ambient OC / EC (but not in OC or EC individually) from 2000 to 2010, confirming increased atmospheric oxidation of OC across the country. Combining the results of emission estimation and observations, the improvement over prior emission inventories is indicated by inter-annual comparisons and correlation analysis. It is also indicated, however, that the estimated growth in emissions might be faster than observed growth, and that some sources with high primary OC / EC, such as burning of biomass, are still underestimated. Further studies to determine changing EFs over time in the residential sector and to compare to other measurements, such as satellite observations, are thus suggested to improve understanding of the levels and trends of primary carbonaceous aerosol emissions in China.

Aerosol chemical characterization and role of carbonaceous aerosol on radiative effect over Varanasi in central Indo-Gangetic Plain

Abstract This study investigates the chemical composition of PM 10 aerosols at Varanasi, in the central Indo-Gangetic Plain (IGP) during April to July 2011, with emphasis on examining the contribution of elemental carbon (EC) to the estimates of direct aerosol radiative effect (DARE). PM 10 samples are analysed for carbonaceous aerosols (Organic Carbon, OC and EC) and water-soluble ionic species (WSIS: Cl − , SO 4 2− , NO 3 − , PO 4 2− NH 4 + , Na + , K + , Mg 2+ and Ca 2+ ) and several diagnostic ratios (OC/EC, K + /EC, etc) have been also used for studying the aerosol sources at Varanasi. PM 10 mass concentration varies between 53 and 310 μg m −3 (mean of 168 ± 73 μg m −3 ), which is much higher than the National and International air quality standards. The OC mass concentration varies from 6 μg m −3 to 24 μg m −3 (mean of 12 ± 5 μg m −3 ; 7% of PM 10 mass), whereas EC ranges between 1.0 and 14.3 μg m −3 (4.4 ± 3.9 μg m −3 ; ∼3% of PM 10 mass). The relative low OC/EC of 3.9 ± 2.0 and strong correlation (R 2 = 0.82) between them suggest the dominance of primary carbonaceous aerosols. The contribution of WSIS to PM 10 is found to be ∼12%, out of which ∼57% and 43% are anions and cations, respectively. The composite DARE estimates via SBDART model reveal significant radiative effect and atmospheric heating rates (0.9–2.3 K day −1 ). Although the EC contributes only ∼3% to the PM 10 mass, its contribution to the surface and atmospheric forcing is significantly high (37–63% and 54–77%, respectively), thus playing a major role in climate implications over Varanasi.

Production-based emissions, consumption-based emissions and consumption-based health impacts of PM2.5 carbonaceous aerosols in Asia

This study determined the production-based emissions, the consumption-based emissions, and the consumption-based health impact of primary carbonaceous aerosols (black carbon: BC, organic carbon: OC) in nine countries and regions in Asia (Indonesia, Malaysia, the Philippines, Singapore, Thailand, China, Taiwan, South Korea, and Japan) in 2008. For the production-based emissions, sectoral emissions inventory of BC and OC for the year of 2008 based on the Asian international input–output tables (AIIOT) was compiled including direct emissions from households. Then, a multiregional environmental input–output analysis with the 2008 AIIOT which was originally developed by updating the table of 2000 was applied for calculating the consumption-based emissions for each country and region. For the production-based emissions, China had the highest BC and OC emissions of 4520 Gg-C in total, which accounted for 75% of the total emissions in the nine countries and regions. For consumption-based emissions, China was estimated to have had a total of 4849 Gg-C of BC and OC emissions, which accounted for 77% of the total emissions in the Asia studied. We also quantified how much countries and regions induced emissions in other countries and regions. Furthermore, taking account of the source–receptor relationships of BC and OC among the countries and regions, we converted their consumption-based emissions into the consumption-based health impact of each country and region. China showed the highest consumption-based health impact of BC and OC totaling 111 × 103 premature deaths, followed by Indonesia, Japan, Thailand and South Korea. China accounted for 87% of the sum total of the consumption-based health impacts of the countries/regions, indicating that China's contribution to consumption-based health impact in Asia was greater than its consumption-based emissions. By elucidating the health impacts that each country and region had on other countries and from which country the impacts were received, we demonstrated that the characteristics of the consumption-based health impact varied significantly by country and region. We also determined the difference in the health impacts to other countries and regions due to the domestic final demand of each country and region, and the health impact due to the domestic final demand of that country or region.

Toward a Minimal Representation of Aerosols in Climate Models: Comparative Decomposition of Aerosol Direct, Semidirect, and Indirect Radiative Forcing

Abstract The authors have decomposed the anthropogenic aerosol radiative forcing into direct contributions from each aerosol species to the planetary energy balance through absorption and scattering of solar radiation, indirect effects of anthropogenic aerosol on solar and infrared radiation through droplet and crystal nucleation on aerosol, and semidirect effects through the influence of solar absorption on the distribution of clouds. A three-mode representation of the aerosol in version 5.1 of the Community Atmosphere Model (CAM5.1) yields global annual mean radiative forcing estimates for each of these forcing mechanisms that are within 0.1 W m−2 of estimates using a more complex seven-mode representation that distinguishes between fresh and aged black carbon and primary organic matter. Simulating fresh black carbon particles separately from internally mixed accumulation mode particles is found to be important only near fossil fuel sources. In addition to the usual large indirect effect on solar radiation, this study finds an unexpectedly large positive longwave indirect effect (because of enhanced cirrus produced by homogenous nucleation of ice crystals on anthropogenic sulfate), small shortwave and longwave semidirect effects, and a small direct effect (because of cancelation and interactions of direct effects of black carbon and sulfate). Differences between the three-mode and seven-mode versions are significantly larger (up to 0.2 W m−2) when the hygroscopicity of primary organic matter is decreased from 0.1 to 0 and transfer of the primary carbonaceous aerosol to the accumulation mode in the seven-mode version requires more hygroscopic material coating the primary particles. Radiative forcing by cloudborne anthropogenic black carbon is only −0.07 W m−2.

Sulfur dioxide and primary carbonaceous aerosol emissions in China and India, 1996–2010

Abstract. China and India are the two largest anthropogenic aerosol generating countries in the world. In this study, we develop a new inventory of sulfur dioxide (SO2) and primary carbonaceous aerosol (i.e., black and organic carbon, BC and OC) emissions from these two countries for the period 1996–2010, using a technology-based methodology. Emissions from major anthropogenic sources and open biomass burning are included, and time-dependent trends in activity rates and emission factors are incorporated in the calculation. Year-specific monthly temporal distributions for major sectors and gridded emissions at a resolution of 0.1°×0.1° distributed by multiple year-by-year spatial proxies are also developed. In China, the interaction between economic development and environmental protection causes large temporal variations in the emission trends. From 1996 to 2000, emissions of all three species showed a decreasing trend (by 9 %–17 %) due to a slowdown in economic growth, a decline in coal use in non-power sectors, and the implementation of air pollution control measures. With the economic boom after 2000, emissions from China changed dramatically. BC and OC emissions increased by 46 % and 33 % to 1.85 Tg and 4.03 Tg in 2010. SO2 emissions first increased by 61 % to 34.0 Tg in 2006, and then decreased by 9.2 % to 30.8 Tg in 2010 due to the wide application of flue-gas desulfurization (FGD) equipment in power plants. Driven by the remarkable energy consumption growth and relatively lax emission controls, emissions from India increased by 70 %, 41 %, and 35 % to 8.81 Tg, 1.02 Tg, and 2.74 Tg in 2010 for SO2, BC, and OC, respectively. Monte Carlo simulations are used to quantify the emission uncertainties. The average 95 % confidence intervals (CIs) of SO2, BC, and OC emissions are estimated to be −16 %–17 %, −43 %–93 %, and −43 %–80 % for China, and −15 %–16 %, −41 %–87 %, and −44 %–92 % for India, respectively. Sulfur content, fuel use, and sulfur retention of hard coal and the actual FGD removal efficiency are the main contributors to the uncertainties of SO2 emissions. Biofuel combustion related parameters (i.e., technology divisions, fuel use, and emission factor determinants) are the largest source of OC uncertainties, whereas BC emissions are also sensitive to the parameters of coal combustion in the residential and industrial sectors and the coke-making process. Comparing our results with satellite observations, we find that the trends of estimated emissions in both China and India are in good agreement with the trends of aerosol optical depth (AOD) and SO2 retrievals obtained from different satellites.

An approach to estimate global biomass burning emissions of organic and black carbon from MODIS fire radiative power

Biomass burning is the main global source of fine primary carbonaceous aerosols in the form of organic carbon (OC) and black carbon (BC). We present an approach to estimate biomass burning aerosol emissions based on the measurement of radiative energy released during combustion. We make use of both Aqua and Terra MODIS observations to estimate the fire radiative energy using a simple model to parameterize the fire diurnal cycle based on the long‐term ratio between Terra and Aqua MODIS FRP. The parameterization is developed using cases of frequent (up to 12 times daily) MODIS observations, geostationary data from SEVIRI, and precessing observations from TRMM VIRS. FRE‐based emission coefficients for the organic and black carbon (OCBC) component of fine mode aerosols are computed from multiple regions encompassing grassland/savanna, tropical forest, and extratropical forest biomes using OCBC emission estimates derived from the MODIS fine mode aerosol product and an inverse aerosol transport model. The values of emission coefficients for OCBC retrieved were 2.7 ± 0.3 g/MJ for grassland/savanna, 8.6 ± 0.8 g/MJ for tropical forest, and 14.4 ± 0.8 g/MJ for extratropical forest. The FRE monthly data are then used to estimate OCBC emissions from biomass burning on a global basis. For 2001 to 2007, our annual estimates are comparable to previously published values. According to our estimate, the OCBC emissions are the largest for 2003 (18.8 Tg), roughly 20% above average and primarily driven by wildland fires in the Lake Baikal region (Russia).

Contribution of primary carbonaceous aerosol to cloud condensation nuclei: processes and uncertainties evaluated with a global aerosol microphysics model

Abstract. This paper explores the impacts of primary carbonaceous aerosol on cloud condensation nuclei (CCN) concentrations in a global climate model with size-resolved aerosol microphysics. Organic matter (OM) and elemental carbon (EC) from two emissions inventories were incorporated into a preexisting model with sulfate and sea-salt aerosol. The addition of primary carbonaceous aerosol increased CCN(0.2%) concentrations by 65–90% in the globally averaged surface layer depending on the carbonaceous emissions inventory used. Sensitivity studies were performed to determine the relative importance of organic solubility/hygroscopicity in predicting CCN. In a sensitivity study where carbonaceous aerosol was assumed to be completely insoluble, concentrations of CCN(0.2%) still increased by 40–50% globally over the no carbonaceous simulation because primary carbonaceous emissions were able to become CCN via condensation of sulfuric acid. This shows that approximately half of the contribution of primary carbonaceous particles to CCN in our model comes from the addition of new particles (seeding effect) and half from the contribution of organic solute (solute effect). The solute effect tends to dominate more in areas where there is less inorganic aerosol than organic aerosol and the seeding effect tends to dominate in areas where there is more inorganic aerosol than organic aerosol. It was found that an accurate simulation of the number size distribution is necessary to predict the CCN concentration but assuming an average chemical composition will generally give a CCN concentration within a factor of 2. If a "typical" size distribution is assumed for each species when calculating CCN, such as is done in bulk aerosol models, the mean error relative to a simulation with size resolved microphysics is on the order of 35%. Predicted values of carbonaceous aerosol mass and aerosol number were compared to observations and the model showed average errors of a factor of 3 for carbonaceous mass and a factor of 4 for total aerosol number; however, errors in the accumulation mode concentrations were found to be lower in comparisons with European and marine observations.. The errors in CN and carbonaceous mass may be reduced by improving the emission size distributions of both primary sulfate and primary carbonaceous aerosol.

Comparison of measurements of peroxyacyl nitrates and primary carbonaceous aerosol concentrations in Mexico City determined in 1997 and 2003

Abstract. The concentrations of peroxyacetyl nitrate (PAN) in ambient air can be a good indicator of air quality and the effectiveness of control strategies for reducing ozone levels in urban areas. As PAN is formed by the oxidation of reactive hydrocarbons in the presence of nitrogen dioxide (NO2), it is a direct measure of the peroxyacyl radical levels produced from reactive organic emissions in the urban air shed. Carbon soot, known as black carbon (BC) or elemental carbon (EC), is a primary atmospheric aerosol species and is a good indicator of the levels of combustion emissions, particularly from diesel engines, in major cities. Mexico City is the second largest megacity in the world and has long suffered from poor air quality. Reported here are atmospheric measurements of PAN and BC obtained in Mexico City during the Mexico Megacity 2003 field study. These results are compared with measurements obtained earlier during the Investigación sobre Materia Particulada y Deterioro Atmosférico – Aerosol and Visibility Research (IMADA-AVER) campaign in 1997 to obtain an estimate of the changes in emissions in Mexico City and the effectiveness of control strategies adopted during that time. Concentrations of PAN in 1997 reached a maximum of 34 ppb with an average daily maximum of 15 ppb. The PAN levels recorded in 2003 were quite different, with an average daily maximum of 3 ppb. This dramatic reduction in PAN levels observed in 2003 indicate that reactive hydrocarbon emissions have been reduced in the city due to controls on olefins in liquefied petroleum gas (LPG) and also due to the significant number of newer vehicles with catalytic converters that have replaced older higher emission vehicles. In contrast, black/elemental carbon levels were similar in 1997 and 2003 indicating little improvement likely due to the lack of controls on diesel vehicles in the city. Thus, while air quality and ozone production have improved, Mexico City and other megacities continue to be a major source of black carbon aerosols, which can be an important species in determining regional radiative balance and climate.

Application of positive matrix factorization in estimating aerosol secondary organic carbon in Hong Kong and its relationship with secondary sulfate

Abstract. Secondary organic carbon (SOC) is often a significant portion of organic carbon (OC) in ambient particulate matter (PM). The levels and seasonal patterns of SOC in Hong Kong were examined using more than 2000 PM10 measurements made over a 4.5-year period (1998–2002) in a network of ten air quality monitoring stations. The positive matrix factorization (PMF) model was used to analyze this large data set for source identification and apportioning. SOC was subsequently estimated to be the sum of OC present in the secondary sources, i.e., secondary sulfate, secondary nitrate, and secondary organic aerosol. The annual average SOC as estimated by the PMF method was 4.25 μg C/m3 while the summer average was 1.66 μg C/m3 and the winter average was 7.05 μg C/m3. In comparison, the method that uses EC as a tracer for primary carbonaceous aerosol sources to derive SOC overestimated SOC by 70–212% for the summer samples and by 4–43% for the winter samples. The overestimation by the EC tracer method resulted from the inability of obtaining a single OC/EC ratio that represented a mixture of primary sources varying in time and space. We found that SOC and secondary sulfate had synchronous seasonal variation and were correlated in individual seasons, suggesting common factors that control their formation. Additionally, the presence of SOC was found to be enhanced more than that of secondary sulfate in the winter. We postulate this to be a combined result of favorable partitioning of semivolatile SOC species in the particle phase and more abundant SOC precursors in the winter.

On the future of carbonaceous aerosol emissions

This paper presents the first model‐based forecasts of future emissions of the primary carbonaceous aerosols, black carbon (BC) and organic carbon (OC). The forecasts build on a recent 1996 inventory of emissions that contains detailed fuel, technology, sector, and world‐region specifications. The forecasts are driven by four IPCC scenarios, A1B, A2, B1, and B2, out to 2030 and 2050, incorporating not only changing patterns of fuel use but also technology development. Emissions from both energy generation and open biomass burning are included. We project that global BC emissions will decline from 8.0 Tg in 1996 to 5.3–7.3 Tg by 2030 and to 4.3–6.1 Tg by 2050, across the range of scenarios. We project that OC emissions will decline from 34 Tg in 1996 to 24–30 Tg by 2030 and to 21–28 Tg by 2050. The introduction of advanced technology with lower emission rates, as well as a shift away from the use of traditional solid fuels in the residential sector, more than offsets the increased combustion of fossil fuels worldwide. Environmental pressures and a diminishing demand for new agricultural land lead to a slow decline in the amount of open biomass burning. Although emissions of BC and OC are generally expected to decline around the world, some regions, particularly South America, northern Africa, the Middle East, South Asia, Southeast Asia, and Oceania, show increasing emissions in several scenarios. Particularly difficult to control are BC emissions from the transport sector, which increase under most scenarios. We expect that the BC/OC emission ratio for energy sources will rise from 0.5 to as much as 0.8, signifying a shift toward net warming of the climate system due to carbonaceous aerosols. When biomass burning is included, however, the BC/OC emission ratios are for the most part invariant across scenarios at about 0.2.

Global modelling of secondary organic aerosol in the troposphere: a sensitivity analysis

Abstract. A global 3-dimensional chemistry/transport model able to describe O3, NOx, Volatile Organic Compounds (VOC), sulphur and NH3 chemistry has been extended to simulate the temporal and spatial distribution of primary and secondary carbonaceous aerosols in the troposphere focusing on Secondary Organic Aerosol (SOA) formation. A number of global simulations have been performed to determine a possible range of annual global SOA production and investigate uncertainties associated with the model results. The studied uncertainties in the SOA budget have been evaluated to be in decreasing importance: the potentially irreversible sticking of the semi-volatile compounds on aerosols, the enthalpy of vaporization of these compounds, the partitioning of SOA on non-carbonaceous aerosols, the conversion of aerosols from hydrophobic to hydrophilic, the emissions of primary carbonaceous aerosols, the chemical fate of the first generation products and finally the activity coefficient of the condensable species. The large uncertainties associated with the emissions of VOC and the adopted simplification of chemistry have not been investigated in this study. Although not all sources of uncertainties have been investigated, according to our calculations, the above factors within the experimental range of variations could result to an overall uncertainty of about a factor of 20 in the global SOA budget. The global annual SOA production from biogenic VOC might range from 2.5 to 44.5 Tg of organic matter per year, whereas that from anthropogenic VOC ranges from 0.05 to 2.62 Tg of organic matter per year. These estimates can be considered as a lower limit, since partitioning on coarse particles like nitrate, dust or sea-salt, together with the partitioning and the dissociation of the semi-volatile products in aerosol water has been neglected. Comparison of model results to observations, where available, shows a better agreement for the upper budget estimates than for the lower ones.