Showing papers on "Particulates published in 2016"

Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China

Abstract: Fine-particle pollution associated with winter haze threatens the health of more than 400 million people in the North China Plain. Sulfate is a major component of fine haze particles. Record sulfate concentrations of up to ~300 μg m −3 were observed during the January 2013 winter haze event in Beijing. State-of-the-art air quality models that rely on sulfate production mechanisms requiring photochemical oxidants cannot predict these high levels because of the weak photochemistry activity during haze events. We find that the missing source of sulfate and particulate matter can be explained by reactive nitrogen chemistry in aerosol water. The aerosol water serves as a reactor, where the alkaline aerosol components trap SO 2 , which is oxidized by NO 2 to form sulfate, whereby high reaction rates are sustained by the high neutralizing capacity of the atmosphere in northern China. This mechanism is self-amplifying because higher aerosol mass concentration corresponds to higher aerosol water content, leading to faster sulfate production and more severe haze pollution.

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.

One-year simulation of ozone and particulate matter in Chinausing WRF/CMAQ modeling system

Abstract: . China has been experiencing severe air pollution in recent decades. Although an ambient air quality monitoring network for criteria pollutants has been constructed in over 100 cities since 2013 in China, the temporal and spatial characteristics of some important pollutants, such as particulate matter (PM) components, remain unknown, limiting further studies investigating potential air pollution control strategies to improve air quality and associating human health outcomes with air pollution exposure. In this study, a yearlong (2013) air quality simulation using the Weather Research and Forecasting (WRF) model and the Community Multi-scale Air Quality (CMAQ) model was conducted to provide detailed temporal and spatial information of ozone (O3), total PM2.5, and chemical components. Multi-resolution Emission Inventory for China (MEIC) was used for anthropogenic emissions and observation data obtained from the national air quality monitoring network were collected to validate model performance. The model successfully reproduces the O3 and PM2.5 concentrations at most cities for most months, with model performance statistics meeting the performance criteria. However, overprediction of O3 generally occurs at low concentration range while underprediction of PM2.5 happens at low concentration range in summer. Spatially, the model has better performance in southern China than in northern China, central China, and Sichuan Basin. Strong seasonal variations of PM2.5 exist and wind speed and direction play important roles in high PM2.5 events. Secondary components have more boarder distribution than primary components. Sulfate (SO42−), nitrate (NO3−), ammonium (NH4+), and primary organic aerosol (POA) are the most important PM2.5 components. All components have the highest concentrations in winter except secondary organic aerosol (SOA). This study proves the ability of the CMAQ model to reproduce severe air pollution in China, identifies the directions where improvements are needed, and provides information for human exposure to multiple pollutants for assessing health effects.

Direct observation of aqueous secondary organic aerosol from biomass-burning emissions.

Abstract: The mechanisms leading to the formation of secondary organic aerosol (SOA) are an important subject of ongoing research for both air quality and climate. Recent laboratory experiments suggest that reactions taking place in the atmospheric liquid phase represent a potentially significant source of SOA mass. Here, we report direct ambient observations of SOA mass formation from processing of biomass-burning emissions in the aqueous phase. Aqueous SOA (aqSOA) formation is observed both in fog water and in wet aerosol. The aqSOA from biomass burning contributes to the “brown” carbon (BrC) budget and exhibits light absorption wavelength dependence close to the upper bound of the values observed in laboratory experiments for fresh and processed biomass-burning emissions. We estimate that the aqSOA from residential wood combustion can account for up to 0.1–0.5 Tg of organic aerosol (OA) per y in Europe, equivalent to 4–20% of the total OA emissions. Our findings highlight the importance of aqSOA from anthropogenic emissions on air quality and climate.

Past, present and future atmospheric nitrogen deposition

Abstract: Reactive nitrogen emissions into the atmosphere are increasing due to human activities, affecting nitrogen deposition to the surface and impacting the productivity of terrestrial and marine ecosystems. An atmospheric chemistry-transport model (TM4-ECPL) is here used to calculate the global distribution of total nitrogen deposition, accounting for the first time for both its inorganic and organic fractions in gaseous and particulate phases, and past and projected changes due to anthropogenic activities. The anthropogenic and biomass burning ACCMIP historical and RCP6.0 and RCP8.5 emissions scenarios are used. Accounting for organic nitrogen (ON) primary emissions, the present-day global nitrogen atmospheric source is about 60% anthropogenic, while total N deposition increases by about 20% relative to simulations without ON primary emissions. About 20-25% of total deposited N is ON. About 10% of the emitted nitrogen oxides are deposited as ON instead of inorganic nitrogen (IN) as is considered in most global models. Almost a 3-fold increase over land (2-fold over the ocean) has been calculated for soluble N deposition due to human activities from 1850 to present. The investigated projections indicate significant changes in the regional distribution of N deposition and chemical composition, with reduced compounds gaining importance relative to oxidized ones, but very small changes in the global total flux. Sensitivity simulations quantify uncertainties due to the investigated model parameterizations of IN partitioning onto aerosols and of N chemically fixed on organics to be within 10% for the total soluble N deposition and between 25-35% for the dissolved ON deposition. Larger uncertainties are associated with N emissions.

Size-resolved source apportionment of particulate matter in urban Beijing during haze and non-haze episodes

Abstract: . Additional size-resolved chemical information is needed before the physicochemical characteristics and sources of airborne particles can be understood; however, this information remains unavailable in most regions of China due to lacking measurement data. In this study, we report observations of various chemical species in size-segregated particle samples that were collected over 1 year in the urban area of Beijing, a megacity that experiences severe haze episodes. In addition to fine particles, high concentrations of coarse particles were measured during the periods of haze. The abundance and chemical compositions of the particles in this study were temporally and spatially variable, with major contributions from organic matter and secondary inorganic aerosols. The contributions of organic matter to the particle mass decreased from 37.9 to 31.2 %, and the total contribution of sulfate, nitrate and ammonium increased from 19.1 to 33.9 % between non-haze and haze days, respectively. Due to heterogeneous reactions and hygroscopic growth, the peak concentrations of the organic carbon, cadmium and sulfate, nitrate, ammonium, chloride and potassium shifted from 0.43 to 0.65 µm on non-haze days to 0.65–1.1 µm on haze days. Although the size distributions of lead and thallium were similar during the observation period, their concentrations increased by a factor of more than 1.5 on haze days compared with non-haze days. We observed that sulfate and ammonium, which have a size range of 0.43–0.65 µm, sulfate and nitrate, which have a size range of 0.65–1.1 µm, calcium, which has a size range of 5.8–9 µm, and the meteorological factors of relative humidity and wind speed were responsible for haze pollution when the visibility was less than 10 km. Source apportionment using Positive Matrix Factorization showed six PM2.1 sources and seven PM2.1–9 common sources: secondary inorganic aerosol (25.1 % for fine particles vs. 9.8 % for coarse particles), coal combustion (17.7 % vs. 7.8 %), biomass burning (11.1 % vs. 11.8 %), industrial pollution (12.1 % vs. 5.1 %), road dust (8.4 % vs. 10.9 %), vehicle emissions (19.6 % for fine particles), mineral dust (22.6 % for coarse particles) and organic aerosol (23.6 % for coarse particles). The contributions of the first four factors and vehicle emissions were higher on haze days than non-haze days, while the reverse is true for road dust and mineral dust. The sources' contribution generally increased as the size decreased, with the exception of mineral dust. However, two peaks were consistently found in the fine and coarse particles. In addition, the sources' contribution varied with the wind direction, with coal and oil combustion products increasing during southern flows. This result suggests that future air pollution control strategies should consider wind patterns, especially during episodes of haze. Furthermore, the findings of this study indicated that the PM2.5-based data set is insufficient for determining source control policies for haze in China and that detailed size-resolved information is needed to characterize the important sources of particulate matter in urban regions and better understand severe haze pollution.

Significant Atmospheric Aerosol Pollution Caused by World Food Cultivation

Abstract: Particulate matter is a major concern for public health, causing cancer and cardiopulmonary mortality. Therefore, governments in most industrialized countries monitor and set limits for particulate matter. To assist policy makers, it is important to connect the chemical composition and severity of particulate pollution to its sources. Here we show how agricultural practices, livestock production, and the use of nitrogen fertilizers impact near-surface air quality. In many densely populated areas, aerosols formed from gases that are released by fertilizer application and animal husbandry dominate over the combined contributions from all other anthropogenic pollution. Here we test reduction scenarios of combustion-based and agricultural emissions that could lower air pollution. For a future scenario, we find opposite trends, decreasing nitrate aerosol formation near the surface while total tropospheric loads increase. This suggests that food production could be increased to match the growing global population without sacrificing air quality if combustion emission is decreased.

Ubiquity of organic nitrates from nighttime chemistry in the European submicron aerosol

Abstract: In the atmosphere nighttime removal of volatile organic compounds is initiated to a large extent by reaction with the nitrate radical (NO3) forming organic nitrates which partition between gas and particulate phase. Here we show based on particle phase measurements performed at a suburban site in the Netherlands that organic nitrates contribute substantially to particulate nitrate and organic mass. Comparisons with a chemistry transport model indicate that most of the measured particulate organic nitrates are formed by NO3 oxidation. Using aerosol composition data from three intensive observation periods at numerous measurement sites across Europe, we conclude that organic nitrates are a considerable fraction of fine particulate matter (PM1) at the continental scale. Organic nitrates represent 34% to 44% of measured submicron aerosol nitrate and are found at all urban and rural sites, implying a substantial potential of PM reduction by NOx emission control.

The Impact of Individual Anthropogenic Emissions Sectors on the Global Burden of Human Mortality due to Ambient Air Pollution

Abstract: Background:Exposure to ozone and fine particulate matter (PM2.5) can cause adverse health effects, including premature mortality due to cardiopulmonary diseases and lung cancer. Recent studies quan...

Characterization of emissions from a desktop 3D printer and indoor air measurements in office settings

Abstract: Emissions from a desktop 3D printer based on fused deposition modeling (FDM) technology were measured in a test chamber and indoor air was monitored in office settings. Ultrafine aerosol (UFA) emissions were higher while printing a standard object with polylactic acid (PLA) than with acrylonitrile butadiene styrene (ABS) polymer (2.1 × 10(9) vs. 2.4 × 10(8) particles/min). Prolonged use of the printer led to higher emission rates (factor 2 with PLA and 4 with ABS, measured after seven months of occasional use). UFA consisted mainly of volatile droplets, and some small (100-300 nm diameter) iron containing and soot-like particles were found. Emissions of inhalable and respirable dust were below the limit of detection (LOD) when measured gravimetrically, and only slightly higher than background when measured with an aerosol spectrometer. Emissions of volatile organic compounds (VOC) were in the range of 10 µg/min. Styrene accounted for more than 50% of total VOC emitted when printing with ABS; for PLA, methyl methacrylate (MMA, 37% of TVOC) was detected as the predominant compound. Two polycyclic aromatic hydrocarbons (PAH), fluoranthene and pyrene, were observed in very low amounts. All other analyzed PAH, as well as inorganic gases and metal emissions except iron (Fe) and zinc (Zn), were below the LOD or did not differ from background without printing. A single 3D print (165 min) in a large, well-ventilated office did not significantly increase the UFA and VOC concentrations, whereas these were readily detectable in a small, unventilated room, with UFA concentrations increasing by 2,000 particles/cm(3) and MMA reaching a peak of 21 µg/m(3) and still being detectable in the room even 20 hr after printing.

The impact of residential combustion emissions on atmospheric aerosol, human health and climate

Abstract: . Combustion of fuels in the residential sector for cooking and heating results in the emission of aerosol and aerosol precursors impacting air quality, human health, and climate. Residential emissions are dominated by the combustion of solid fuels. We use a global aerosol microphysics model to simulate the impact of residential fuel combustion on atmospheric aerosol for the year 2000. The model underestimates black carbon (BC) and organic carbon (OC) mass concentrations observed over Asia, Eastern Europe, and Africa, with better prediction when carbonaceous emissions from the residential sector are doubled. Observed seasonal variability of BC and OC concentrations are better simulated when residential emissions include a seasonal cycle. The largest contributions of residential emissions to annual surface mean particulate matter (PM2.5) concentrations are simulated for East Asia, South Asia, and Eastern Europe. We use a concentration response function to estimate the human health impact due to long-term exposure to ambient PM2.5 from residential emissions. We estimate global annual excess adult (> 30 years of age) premature mortality (due to both cardiopulmonary disease and lung cancer) to be 308 000 (113 300–497 000, 5th to 95th percentile uncertainty range) for monthly varying residential emissions and 517 000 (192 000–827 000) when residential carbonaceous emissions are doubled. Mortality due to residential emissions is greatest in Asia, with China and India accounting for 50 % of simulated global excess mortality. Using an offline radiative transfer model we estimate that residential emissions exert a global annual mean direct radiative effect between −66 and +21 mW m−2, with sensitivity to the residential emission flux and the assumed ratio of BC, OC, and SO2 emissions. Residential emissions exert a global annual mean first aerosol indirect effect of between −52 and −16 mW m−2, which is sensitive to the assumed size distribution of carbonaceous emissions. Overall, our results demonstrate that reducing residential combustion emissions would have substantial benefits for human health through reductions in ambient PM2.5 concentrations.

Brown carbon aerosols from burning of boreal peatlands: microphysical properties, emission factors, and implications for direct radiative forcing

Abstract: . The surface air warming over the Arctic has been almost twice as much as the global average in recent decades. In this region, unprecedented amounts of smoldering peat fires have been identified as a major emission source of climate-warming agents. While much is known about greenhouse gas emissions from these fires, there is a knowledge gap on the nature of particulate emissions and their potential role in atmospheric warming. Here, we show that aerosols emitted from burning of Alaskan and Siberian peatlands are predominantly brown carbon (BrC) – a class of visible light-absorbing organic carbon (OC) – with a negligible amount of black carbon content. The mean fuel-based emission factors for OC aerosols ranged from 3.8 to 16.6 g kg−1. Their mass absorption efficiencies were in the range of 0.2–0.8 m2 g−1 at 405 nm (violet) and dropped sharply to 0.03–0.07 m2 g−1 at 532 nm (green), characterized by a mean Angstrom exponent of ≈ 9. Electron microscopy images of the particles revealed their morphologies to be either single sphere or agglomerated “tar balls”. The shortwave top-of-atmosphere aerosol radiative forcing per unit optical depth under clear-sky conditions was estimated as a function of surface albedo. Only over bright surfaces with albedo greater than 0.6, such as snow cover and low-level clouds, the emitted aerosols could result in a net warming (positive forcing) of the atmosphere.

Public Health Costs of Primary PM2.5 and Inorganic PM2.5 Precursor Emissions in the United States

Abstract: Current methods of estimating the public health effects of emissions are computationally too expensive or do not fully address complex atmospheric processes, frequently limiting their applications to policy research. Using a reduced-form model derived from tagged chemical transport model (CTM) simulations, we present PM2.5 mortality costs per tonne of inorganic air pollutants with the 36 km × 36 km spatial resolution of source location in the United States, providing the most comprehensive set of such estimates comparable to CTM-based estimates. Our estimates vary by 2 orders of magnitude. Emission-weighted seasonal averages were estimated at $88,000–130,000/t PM2.5 (inert primary), $14,000–24,000/t SO2, $3,800–14,000/t NOx, and $23,000–66,000/t NH3. The aggregate social costs for year 2005 emissions were estimated at $1.0 trillion dollars. Compared to other studies, our estimates have similar magnitudes and spatial distributions for primary PM2.5 but substantially different spatial patterns for precursor...

Analysis of particulate emissions from tropical biomass burning using aglobal aerosol model and long-term surface observations

Abstract: . We use the GLOMAP global aerosol model evaluated against observations of surface particulate matter (PM2.5) and aerosol optical depth (AOD) to better understand the impacts of biomass burning on tropical aerosol over the period 2003 to 2011. Previous studies report a large underestimation of AOD over regions impacted by tropical biomass burning, scaling particulate emissions from fire by up to a factor of 6 to enable the models to simulate observed AOD. To explore the uncertainty in emissions we use three satellite-derived fire emission datasets (GFED3, GFAS1 and FINN1). In these datasets the tropics account for 66–84 % of global particulate emissions from fire. With all emission datasets GLOMAP underestimates dry season PM2.5 concentrations in regions of high fire activity in South America and underestimates AOD over South America, Africa and Southeast Asia. When we assume an upper estimate of aerosol hygroscopicity, underestimation of AOD over tropical regions impacted by biomass burning is reduced relative to previous studies. Where coincident observations of surface PM2.5 and AOD are available we find a greater model underestimation of AOD than PM2.5, even when we assume an upper estimate of aerosol hygroscopicity. Increasing particulate emissions to improve simulation of AOD can therefore lead to overestimation of surface PM2.5 concentrations. We find that scaling FINN1 emissions by a factor of 1.5 prevents underestimation of AOD and surface PM2.5 in most tropical locations except Africa. GFAS1 requires emission scaling factor of 3.4 in most locations with the exception of equatorial Asia where a scaling factor of 1.5 is adequate. Scaling GFED3 emissions by a factor of 1.5 is sufficient in active deforestation regions of South America and equatorial Asia, but a larger scaling factor is required elsewhere. The model with GFED3 emissions poorly simulates observed seasonal variability in surface PM2.5 and AOD in regions where small fires dominate, providing independent evidence that GFED3 underestimates particulate emissions from small fires. Seasonal variability in both PM2.5 and AOD is better simulated by the model using FINN1 emissions. Detailed observations of aerosol properties over biomass burning regions are required to better constrain particulate emissions from fires.

Contribution of ship emissions to the concentration and deposition of air pollutants in Europe

Abstract: . Emissions from the marine transport sector are one of the least-regulated anthropogenic emission sources and contribute significantly to air pollution. Although strict limits were introduced recently for the maximum sulfur content in marine fuels in the SECAs (sulfur emission control areas) and in EU ports, sulfur emissions outside the SECAs and emissions of other components in all European maritime areas have continued to increase in the last two decades. We have used the air quality model CAMx (Comprehensive Air Quality Model with Extensions) with and without ship emissions for the year 2006 to determine the effects of international shipping on the annual as well as seasonal concentrations of ozone, primary and secondary components of PM2.5, and the dry and wet deposition of nitrogen and sulfur compounds in Europe. The largest changes in pollutant concentrations due to ship emissions were predicted for summer. Concentrations of particulate sulfate increased due to ship emissions in the Mediterranean (up to 60 %), the English Channel and the North Sea (30–35 %), while increases in particulate nitrate levels were found especially in the north, around the Benelux area (20 %), where there were high NH3 land-based emissions. Our model results showed that not only are the atmospheric concentrations of pollutants affected by ship emissions, but also depositions of nitrogen and sulfur compounds increase significantly along the shipping routes. NOx emissions from the ships, especially in the English Channel and the North Sea, cause a decrease in the dry deposition of reduced nitrogen at source regions by moving it from the gas phase to the particle phase which then contributes to an increase in the wet deposition at coastal areas with higher precipitation. In the western Mediterranean region, on the other hand, model results show an increase in the deposition of oxidized nitrogen (mostly HNO3) due to the ship traffic. Dry deposition of SO2 seems to be significant along the shipping routes, whereas sulfate wet deposition occurs mainly along the Scandinavian and Adriatic coasts. The results presented in this paper suggest that evolution of NOx emissions from ships and land-based NH3 emissions will play a significant role in future European air quality.

Characteristics of aerosol pollution during heavy haze events in Suzhou, China

Abstract: . Extremely severe haze weather events occurred in many cities in China, especially in the east part of the country, in January 2013. Comprehensive measurements including hourly concentrations of PM2.5 and its major chemical components (water-soluble inorganic ions, organic carbon (OC), and elemental carbon (EC)) and related gas-phase precursors were conducted via an online monitoring system in Suzhou, a medium-sized city in Jiangsu province, just east of Shanghai. PM2.5 (particulate matter with an aerodynamic diameter of 2.5 µm or less) frequently exceeded 150 µg m−3 on hazy days, with the maximum reaching 324 µg m−3 on 14 January 2013. Unfavorable weather conditions (high relative humidity (RH), and low rainfall, wind speed, and atmospheric pressure) were conducive to haze formation. High concentrations of secondary aerosol species (including SO42−, NO3−, NH4+, and SOC) and gaseous precursors were observed during the first two haze events, while elevated primary carbonaceous species emissions were found during the third haze period, pointing to different haze formation mechanisms. Organic matter (OM), (NH4)2SO4, and NH4NO3 were found to be the major contributors to visibility impairment. High concentrations of sulfate and nitrate might be explained by homogeneous gas-phase reactions under low RH conditions and by heterogeneous processes under relatively high RH conditions. Analysis of air mass trajectory clustering and potential source contribution function showed that aerosol pollution in the studied areas was mainly caused by local activities and surrounding sources transported from nearby cities.

Sub-micrometre particulate matter is primarily in liquid form over Amazon rainforest

Abstract: The physical state of atmospheric particulate matter affects its growth and reactivity, which can affect climate. Measurements of particle rebound reveal that particulate matter over the Amazon forest is usually liquid during wet and dry seasons.