Application of a Lagrangian particle model to assess the impact of harbour,industrial and urban activities on air quality in the Taranto area,Italy

This paper evaluates the relative impact on air quality of harbour emissions, with respect to other emission sources located in the same area. The impact assessment study was conducted in the city of Taranto, Italy. This area was considered as representative of a typical Mediterranean harbour region, where shipping, industries and urban activities co-exist at a short distance, producing an ideal case to study the interaction among these different sources. Chemical and meteorological field campaigns were carried out to provide data to this study. An emission inventory has been developed taking into account industrial sources, traffic, domestic heating, fugitive and harbour emissions. A 3D Lagrangian particle dispersion model (SPRAY) has then been applied to the study area using reconstructed meteorological fields calculated by the diagnostic meteorological model MINERVE. 3D short term hourly concentrations have been computed for both all and specific sources. Industrial activities are found to be the main contributor to SO₂. Industry and traffic emissions are mainly responsible for NO_x simulated concentrations. CO concentrations are found to be mainly related to traffic emissions, while primary PM₁₀ simulated concentrations tend to be linked to industrial and fugitive emissions. Contributions of harbour activities to the seasonal average concentrations of SO₂ and NO_x are predicted to be up to 5 and 30 μg m⁻³, respectively to be compared to a overall peak values of 60 μg m⁻³ for SO₂ and 70 μg m⁻³ for NO_x. At selected urban monitoring stations, SO₂ and NO_x average source contributions are predicted to be both of about 9% from harbour activities, while 87% and 41% respectively of total concentrations are predicted to be of industrial origin.     

Decadal reductions of traffic emissions on a transit route in Austria – results of the Tauerntunnel experiment 1997

Real-world emissions of a traffic fleet on a transit route in Austria were determined in the Tauerntunnel experiment in October 1997. The total number of vehicles and the average speed was nearly the same on both measuring days (465 vehicles 30 min⁻¹ and 76 km h⁻¹ on the workday, 477 and 78 km h⁻¹ on Sunday). The average workday fleet contained 17.6% heavy-duty vehicles (HDV) and the average Sunday fleet 2.8% HDV resulting in up to four times higher emission rates per vehicle per km on the workday than on Sunday for most of the regulated components (CO₂, CO, NO_x, SO₂, and particulate matter-PM10). Emission rates of NMVOC accounted for 200 mg vehicle⁻¹ km⁻¹ on both days. The relative contributions of light-duty vehicles (LDV) and HDV to the total emissions indicated that aldehydes, BTEX (benzene, toluene, ethylbenzene, xylenes), and alkanes are mainly produced by LDV, while HDV dominated emissions of CO, NO_x, SO₂, and PM10. Emissions of NO_x caused by HDV were 16,100 mg vehicle⁻¹ km⁻¹ (as NO₂). Produced by LDV they were much lower at 360 mg vehicle⁻¹ km⁻¹. Comparing the emission rates to the results that were obtained by the 1988 experiment at the same place significant changes in the emission levels of hydrocarbons and CO, which accounted 1997 to only 10% of the levels in 1988, were noticed. However, the decrease of PM has been modest leading to values of 80 and 60% of the levels in 1988 on the workday and on Sunday, respectively. Emission rates of NO_x determined on the workday in 1997 were 3130 mg vehicle⁻¹ km⁻¹ and even higher than in 1988 (2630 mg vehicle⁻¹ km⁻¹), presumable due to the increase of the HD-traffic.     

Assessment of air quality benefits from national air pollution control policies in China. Part II: Evaluation of air quality predictions and air quality benefits assessment

Following the meteorological evaluation in Part I, this Part II paper presents the statistical evaluation of air quality predictions by the U.S. Environmental Protection Agency (U.S. EPA)’s Community Multi-Scale Air Quality (Models-3/CMAQ) model for the four simulated months in the base year 2005. The surface predictions were evaluated using the Air Pollution Index (API) data published by the China Ministry of Environmental Protection (MEP) for 31 capital cities and daily fine particulate matter (PM_2.5, particles with aerodiameter less than or equal to 2.5 μm) observations of an individual site in Tsinghua University (THU). To overcome the shortage in surface observations, satellite data are used to assess the column predictions including tropospheric nitrogen dioxide (NO₂) column abundance and aerosol optical depth (AOD). The result shows that CMAQ gives reasonably good predictions for the air quality.The air quality improvement that would result from the targeted sulfur dioxide (SO₂) and nitrogen oxides (NO_x) emission controls in China were assessed for the objective year 2010. The results show that the emission controls can lead to significant air quality benefits. SO₂ concentrations in highly polluted areas of East China in 2010 are estimated to be decreased by 30–60% compared to the levels in the 2010 Business-As-Usual (BAU) case. The annual PM_2.5 can also decline by 3–15 μg m^?3 (4–25%) due to the lower SO₂ and sulfate concentrations. If similar controls are implemented for NO_x emissions, NO_x concentrations are estimated to decrease by 30–60% as compared with the 2010 BAU scenario. The annual mean PM_2.5 concentrations will also decline by 2–14 μg m^?3 (3–12%). In addition, the number of ozone (O₃) non-attainment areas in the northern China is projected to be much lower, with the maximum 1-h average O₃ concentrations in the summer reduced by 8–30 ppb.     

Establishment of a database of emission factors for atmospheric pollutants from Chinese coal-fired power plants

Field measurements and data investigations were conducted for developing an emission factor database for inventories of atmospheric pollutants from Chinese coal-fired power plants. Gaseous pollutants and particulate matter (PM) of different size fractions were measured using a gas analyzer and an electric low-pressure impactor (ELPI), respectively, for ten units in eight coal-fired power plants across the country. Combining results of field tests and literature surveys, emission factors with 95% confidence intervals (CIs) were calculated by boiler type, fuel quality, and emission control devices using bootstrap and Monte Carlo simulations. The emission factor of uncontrolled SO₂ from pulverized combustion (PC) boilers burning bituminous or anthracite coal was estimated to be 18.0S kg t^?1 (i.e., 18.0 × the percentage sulfur content of coal, S) with a 95% CI of 17.2S–18.5S. NO_X emission factors for pulverized-coal boilers ranged from 4.0 to 11.2 kg t^?1, with uncertainties of 14–45% for different unit types. The emission factors of uncontrolled PM_2.5, PM₁₀, and total PM emitted by PC boilers were estimated to be 0.4A (where A is the percentage ash content of coal), 1.5A and 6.9A kg t^?1, respectively, with 95% CIs of 0.3A–0.5A, 1.1A–1.9A and 5.8A–7.9A. The analogous PM values for emissions with electrostatic precipitator (ESP) controls were 0.032A (95% CI: 0.021A–0.046A), 0.065A (0.039A–0.092A) and 0.094A (0.0656A–0.132A) kg t^?1, and 0.0147A (0.0092–0.0225A), 0.0210A (0.0129A–0.0317A), and 0.0231A (0.0142A–0.0348A) for those with both ESP and wet flue-gas desulfurization (wet-FGD). SO₂ and NO_X emission factors for Chinese power plants were smaller than those of U.S. EPA AP-42 database, due mainly to lower heating values of coals in China. PM emission factors for units with ESP, however, were generally larger than AP-42 values, because of poorer removal efficiencies of Chinese dust collectors. For units with advanced emission control technologies, more field measurements are needed to reduce emission factor uncertainties.     

Quantification on source/receptor relationship of primary pollutants and secondary aerosols from ground sources—Part I. Theory

A new algorithm has been derived for trajectory models to determine the transfer coefficient of each source along or adjacent to a trajectory and to calculate the concentrations of SO₂, NO_x, sulfate, nitrate, fine particulate matter (PM) and coarse PM at a receptor. The transfer coefficient t_f (s m⁻¹) is defined to be the ratio between the contributed concentration ΔC (μg m⁻³) to the receptor from a ground source and the emission rate of the source q (μg m⁻² s⁻¹) at a grid, i.e. t_f≡ΔC/q. The model is developed by combining with a backward trajectory scheme and a circuit-type's parameterization. First, the transfer coefficients of grids along or adjacent a back-trajectory are calculated. Then, the contributed concentration of each emission grid is determined by multiplying its emission rate with the transfer coefficient of the grid. Finally, the concentration at the receptor is determined by the summation of all the contributed concentrations within the domain of simulation.     

Aircraft measurements of O3, NOx,CO, VOCs,and SO2 in the Yangtze River Delta region

In this study, air pollutants, including ozone (O₃), nitrogen oxides (NO_x = NO + NO₂), carbon monoxides (CO), sulfur dioxide (SO₂), and volatile organic compounds (VOCs) measured in the Yangtze River Delta (YRD) region during several air flights between September/30 and October/11 are analyzed. This measurement provides horizontal and vertical distributions of air pollutants in the YRD region. The analysis of the result shows that the measured O₃ concentrations range from 20 to 60 ppbv. These values are generally below the US national standard (84 ppbv), suggesting that at the present, the O₃ pollutions are modest in this region. The NO_x concentrations have strong spatial and temporal variations, ranging from 3 to 40 ppbv. The SO₂ concentrations also have large spatial and temporal variations, ranging from 1 to 35 ppbv. The high concentrations of CO are measured with small variations, ranging from 3 to 7 ppmv. The concentrations of VOCs are relatively low, with the total VOC concentrations of less than 6 ppbv. The relative small VOC concentrations and the relative large NO_x concentrations suggest that the O₃ chemical formation is under a strong VOC-limited regime in the YRD region. The measured O₃ and NO_x concentrations are strongly anti-correlated, indicating that enhancement in NO_x concentrations leads to decrease in O₃ concentrations. Moreover, the O₃ concentrations are more sensitive to NO_x concentrations in the rural region than in the city region. The ratios of Δ[O₃]/Δ[NO_x] are ?2.3 and ?0.25 in the rural and in the city region, respectively. In addition, the measured NO_x and SO₂ concentrations are strongly correlated, highlighting that the NO_x and SO₂ are probably originated from same emission sources. Because SO₂ emissions are significantly originated from coal burnings, the strong correlation between SO₂ and NO_x concentrations suggests that the NO_x emission sources are mostly from coal burned sources. As a result, the future automobile increases could lead to rapid enhancements in O₃ concentrations in the YRD region.     

The water-soluble ionic composition of PM2.5 in Shanghai and Beijing,China

A year-long field study to characterize the ionic species in PM2.5 was carried out in Shanghai and Beijing, China, in 1999–2000. Weekly samples of PM2.5 were collected using a special low flow rate (0.4 l min⁻¹) sampler. In Shanghai, SO₄²⁻ NO₃⁻ and NH₄⁺ were the dominant ionic species, which accounted for 46%, 18% and 17% of the total mass of ions, respectively. Local SO₂ emissions were an important source of SO₄²⁻ in PM2.5 because the SO₄²⁻ concentration was correlated with the SO₂ concentration (r=0.66). The relatively stable SO₄²⁻/SO₂ mass ratio over a large range of temperatures suggests that gas-phase oxidation of SO₂ played a minor role in the formation of SO₄²⁻. The sum of SO₄²⁻ and NO₃⁻ was highly correlated with NH₄⁺ (r=0.96), but insufficient ammonium was present to totally neutralize the aerosol. In Beijing, SO₄²⁻, NO₃⁻ and NH₄⁺ were also the dominant ionic species, constituting 44%, 25% and 16% of the total mass of water-soluble ions, respectively. Local SO₂ emissions were an important source of SO₄²⁻ in the winter since SO₄²⁻ was correlated with SO₂ (r=0.83). The low-mass SO₄²⁻/SO₂ ratio (0.27) during winter, which had low humidity, suggests that gas-phase oxidation of SO₂ was a major route of sulfate formation. In the summer, however, much higher mass ratios of SO₄²⁻/SO₂ (5.6) were observed and were ascribed to in-cloud sulfate formation. The annual average ratio of NO₃⁻/SO₄²⁻ was 0.4 and 0.6 in Shanghai and in Beijing, respectively, suggesting that stationary emissions were still a dominant source in these two cities.     

PM2.5–10, PM2.5 and associated water-soluble inorganic species at a coastal urban site in the metropolitan region of Rio de Janeiro

The concentrations of PM_2.5−10, PM_2.5 and associated water-soluble inorganic species (WSIS) were determined in a coastal site of the metropolitan region of Rio de Janeiro, Southeastern Brazil, from October 1998 to September 1999 (n=50). Samples were dissolved in water and analyzed for major inorganic ions. The mean (± standard deviation; median) concentrations of PM_2.5−10 and PM_2.5 were, respectively, 26 (± 16; 21) μg m⁻³ and 17 (± 13; 14) μg m⁻³. Their mean concentrations were 1.7–1.8 times higher in dry season (May–October) than in rainy season (November–April). The WSIS comprised, respectively, 34% and 28% of the PM_2.5−10 and PM_2.5 masses. Chloride, Na⁺ and Mg²⁺ were the predominant ions in PM_2.5−10, indicating a significant influence of sea-salt aerosols. In PM_2.5, SO₄²⁻ (∼97% nss-SO₄²⁻) and NH₄⁺ were the most abundant ions and their equivalent concentration ratio (SO₄²⁻/NH₄⁺ ∼1.0) suggests that they were present as (NH₄)₂SO₄ particles. The mean concentration of (NH₄)₂SO₄ was 3.4 μg m⁻³. The mean equivalent PM_2.5 NO₃⁻ concentration was eight times smaller than those of SO₄²⁻ and NH₄⁺. The PM_2.5 NO₃⁻ concentration in dry season was three times higher than in rainy season, probably due to reaction of NaCl (sea salt) with HNO₃ as a result of higher levels of NO_y during the dry season and/or reduced volatilization of NH₄NO₃ due to lower wintertime temperature. Chloride depletion was observed in both size ranges, although more pronouncely in PM_2.5.     

Multi-year hourly PM2.5 carbon measurements in New York: Diurnal,day of week and seasonal patterns

Multi-year hourly measurements of PM_2.5 elemental carbon (EC) and organic carbon (OC) from a site in the South Bronx, New York were used to examine diurnal, day of week and seasonal patterns. The hourly carbon measurements also provided temporally resolved information on sporadic EC spikes observed predominantly in winter. Furthermore, hourly EC and OC data were used to provide information on secondary organic aerosol formation. Average monthly EC concentrations ranged from 0.5 to 1.4 μg m^?3 with peak hourly values of several μg m^?3 typically observed from November to March. Mean EC concentrations were lower on weekends (approximately 27% lower on Saturday and 38% lower on Sunday) than on weekdays (Monday to Friday). The weekday/weekend difference was more pronounced during summer months and less noticeable during winter. Throughout the year EC exhibited a similar diurnal pattern to NO_x showing a pronounced peak during the morning commute period (7–10 AM EST). These patterns suggest that EC was impacted by local mobile emissions and in addition by emissions from space heating sources during winter months. Although EC was highly correlated with black carbon (BC) there was a pronounced seasonal BC/EC gradient with summer BC concentrations approximately a factor of 2 higher than EC. Average monthly OC concentrations ranged from 1.0 to 4.1 μg m^?3 with maximum hourly concentrations of 7–11 μg m^?3 predominantly in summer or winter months. OC concentrations generally correlated with PM_2.5 total mass and aerosol sulfate and with NO_x during winter months. OC showed no particular day of week pattern. The OC diurnal pattern was typically different than EC except in winter when OC tracked EC and NO_x indicating local primary emissions contributed significantly to OC during winter at the urban location. On average secondary organic aerosol was estimated to account for 40–50% of OC during winter and up to 63–73% during summer months.     

Analysis of model responses to emission-reduction scenarios within the CityDelta project

This paper investigates how air quality models applied at different scales (50 and 5 km horizontal resolutions) can predict pollution levels in response to emission control strategies in various cities in Europe. This study, involving five modelling teams and focused on four European cities, has been conducted within the CityDelta project (http://aqm.jrc.it/citydelta). The CityDelta models generally agree, on the O₃ changes expected from scenarios representative of the current legislation on air pollution in 2010, named CLE. They also agree about less scope for further improvements from emission controls beyond CLE. For PM₁₀, more significant differences between the models are observed, especially between models with different spatial resolutions. However, these differences are city-dependent and are larger in complex geographical areas such as Milan in the Pô Valley than in the Paris area.Fine scale models generally capture important urban scale effects, which are not represented by regional scale models. For instance, they improve the simulation of potential O₃ increase caused by NO_x emissions reduction in NMVOC-limited regime situations. Large scale models generally underpredict PM mean concentrations in city areas. A series of emission scenarios to address the question of the efficiency of local emission controls designed independently from regional measures is analyzed. The analysis of the CityDelta results contributes to the quantification of the impact of grid resolution in air quality modelling, and its application to emission control scenarios.     

Sub-region (district) and sector level SO2 and NOx emissions for India: assessment of inventories and mitigation flexibility

Sub-regional and sector level distribution of SO₂ and NO_x emissions inventories for India have been estimated for all the 466 Indian districts using base data for years 1990 and 1995. Although, national level emissions provide general guidelines for assessing mitigation alternatives, but significant regional and sectoral variability exist in Indian emissions. Districts reasonably capture this variability to a fine grid as 80% of these districts are smaller than 1°×1° resolution with 60% being smaller than even 1/2°×1/2°. Moreover, districts in India have well-established administrative and institutional mechanisms that would be useful for implementing and monitoring measures. District level emission estimates thus offer a finer regional scale inventory covering the combined interests of the scientific community and policy makers. The inventory assessment methodology adopted is similar to that prescribed by the Intergovernmental Panel on Climate Change (IPCC) for greenhouse gas (GHG) emissions. The sectoral decomposition at district level includes emissions from fossil fuel combustion, non-energy emissions from industrial activities and agriculture. Total SO₂ and NO_x emissions from India were 3542 and 2636 Gg, respectively (1990) and 4638 and 3462 Gg (1995) growing at annual rate of around 5.5%. The sectoral composition of SO₂ emissions indicates a predominance of electric power generation sector (46%). Power and transport sector emissions equally dominate NO_x emissions contributing nearly 30% each. However, majority of power plants are situated in predominantly rural districts while the latter are concentrated in large urban centers. Mitigation efforts for transport sector NO_x emissions would therefore be higher. The district level analysis indicates diverse spatial distribution with the top 5% emitting districts contributing 46.5 and 33.3% of total national SO₂ and NO_x emissions, respectively. This skewed emission pattern, with a few districts, sectors and point sources emitting significant SO₂ and NO_x, offers mitigation flexibility to policy makers for cost-effective mitigation.     

Spatial patterns of mobile source particulate matter emissions-to-exposure relationships across the United States

Assessing the public health benefits from air pollution control measures is assisted by understanding the relationship between mobile source emissions and subsequent fine particulate matter (PM_2.5) exposure. Since this relationship varies by location, we characterized its magnitude and geographic distribution using the intake fraction (iF) concept. We considered emissions of primary PM_2.5 as well as particle precursors SO₂ and NO_x from each of 3080 counties in the US. We modeled the relationship between these emissions and total US population exposure to PM_2.5, making use of a source–receptor matrix developed for health risk assessment. For primary PM_2.5, we found a median iF of 1.2 per million, with a range of 0.12–25. Half of the total exposure was reached by a median distance of 150 km from the county where mobile source emissions originated, though this spatial extent varied across counties from within the county borders to 1800 km away. For secondary ammonium sulfate from SO₂ emissions, the median iF was 0.41 per million (range: 0.050–10), versus 0.068 per million for secondary ammonium nitrate from NO_x emissions (range: 0.00092–1.3). The median distance to half of the total exposure was greater for secondary PM_2.5 (450 km for sulfate, 390 km for nitrate). Regression analyses using exhaustive population predictors explained much of the variation in primary PM_2.5 iF (R²=0.83) as well as secondary sulfate and nitrate iF (R²=0.74 and 0.60), with greater near-source contribution for primary than for secondary PM_2.5. We conclude that long-range dispersion models with coarse geographic resolution are appropriate for risk assessments of secondary PM_2.5 or primary PM_2.5 emitted from mobile sources in rural areas, but that more resolved dispersion models are warranted for primary PM_2.5 in urban areas due to the substantial contribution of near-source populations.     

Predictive NOx emission monitoring on board a passenger ferry

NO_x emissions from a medium speed diesel engine on board a servicing passenger ferry have been indirectly measured using a predictive emission monitoring system (PEMS) over a 1-yr period. Conventional NO_x measurements were carried out with a continuous emission monitoring system (CEMS) at the start of the study to provide historical data for the empirical PEMS function. On three other occasions during the year the CEMS was also used to verify the PEMS and follow any changes in emission signature of the engine. The PEMS consisted of monitoring exhaust O₂ concentrations (in situ electrochemical probe), engine load, combustion air temperature and humidity, and barometric pressure. Practical experiences with the PEMS equipment were positive and measurement data were transferred to a land-based office by using a modem data communication system. The initial PEMS function (PEMS1) gave systematic differences of 1.1–6.9% of the calibration domain (0–1725 ppm) and a relative accuracy of 6.7% when compared with CEMS for whole journeys and varying load situations. Further improvements on the performance could be obtained by updating this function. The calculated yearly emission for a total engine running time of 4618 h was 316 t NO_x±38 t and the average NO_x emission corrected for ambient conditions 14.3 g kWh_corr⁻¹. The exhaust profile of the engine in terms of NO_x, CO and CO₂ emissions as determined by CEMS was similar for most of the year. Towards the end of the study period, a significantly lower NO_x emission was detected which was probably caused by replacement of fuel injector nozzles. The study suggests that PEMS can be a viable option for continuous, long-term NO_x measurements on board ships.     

Nitrogen oxide fluxes between corn (Zea mays L.) leaves and the atmosphere

In the United States, fertilized corn fields, which make up approximately 5% of the total land area, account for approximately 45% of total soil NO_x emissions. Leaf chamber measurements were conducted of NO and NO₂ fluxes between individual corn leaves and the atmosphere in (1) field-grown plants near Champaign, IL (USA) in order to assess the potential role of corn canopies in mitigating soil–NO_x emissions to the atmosphere, and (2) greenhouse-grown plants in order to study the influence of various environmental variables and physiological factors on the dynamics of NO₂ flux. In field-grown plants, fluxes of NO were small and inconsistent from plant to plant. At ambient NO concentrations between 0.1 and 0.3 ppbv, average fluxes were zero. At ambient NO concentrations above 1 ppbv, NO uptake occurred, but fluxes were so small (14.3±0.0 pmol m⁻² s⁻¹) as to be insignificant in the NO_x inventory for this site. In field-grown plants, NO₂ was emitted to the atmosphere at ambient NO₂ concentrations below 0.9 ppbv (the NO₂ compensation point), with the highest rate of emission being 50 pmol m⁻² s⁻¹ at 0.2 ppbv. NO₂ was assimilated by corn leaves at ambient NO₂ concentrations above 0.9 ppbv, with the maximum observed uptake rate being 643 pmol m⁻² s⁻¹ at 6 ppbv. When fluxes above 0.9 ppbv are standardized for ambient NO₂ concentration, the resultant deposition velocity was 1.2±0.1 mm s⁻¹. When scaled to the entire corn canopy, NO₂ uptake rates can be estimated to be as much as 27% of the soil-emitted NO_x. In greenhouse-grown and field-grown leaves, NO₂ deposition velocity was dependent on incident photosynthetic photon flux density (PPFD; 400–700 nm), whether measured above or below the NO₂ compensation point. The shape of the PPFD dependence, and its response to ambient humidity in an experiment with greenhouse-grown plants, led to the conclusion that stomatal conductance is a primary determinant of the PPFD response. However, in field-grown leaves, measured NO₂ deposition velocities were always lower than those predicted by a model solely dependent on stomatal conductance. It is concluded that NO₂ uptake rate is highest when N availability is highest, not when the leaf deficit for N is highest. It is also concluded that the primary limitations to leaf-level NO₂ uptake concern both stomatal and mesophyll components.     

Inventory of aerosol and sulphur dioxide emissions from India. Part II—biomass combustion

A spatially resolved biomass burning data set, and related emissions of sulphur dioxide and aerosol chemical constituents was constructed for India, for 1996–1997 and extrapolated to the INDOEX period (1998–1999). Sources include biofuels (wood, crop waste and dung-cake) and forest fires (accidental, shifting cultivation and controlled burning). Particulate matter (PM) emission factors were compiled from studies of Indian cooking stoves and from literature for open burning. Black carbon (BC) and organic matter (OM) emissions were estimated from these, accounting for combustion temperatures in cooking stoves. Sulphur dioxide emission factors were based on fuel sulphur content and reported literature measurements. Biofuels accounted 93% of total biomass consumption (577 MT yr⁻¹), with forest fires contributing only 7%. The national average biofuel mix was 56 : 21 : 23% of fuelwood, crop waste and dung-cake, respectively. Compared to fossil fuels, biomass combustion was a minor source of SO₂ (7% of total), with higher emissions from dung-cake because of its higher sulphur content. PM_2.5 emissions of 2.04 Tg yr⁻¹ with an “inorganic fraction” of 0.86 Tg yr⁻¹ were estimated. Biomass combustion was the major source of carbonaceous aerosols, accounting 0.25 Tg yr⁻¹ of BC (72% of total) and 0.94 Tg yr⁻¹ of OM (76% of total). Among biomass, fuelwood and crop waste were primary contributors to BC emissions, while dung-cake and forest fires were primary contributors to OM emissions. Northern and the east-coast India had high densities of biomass consumption and related emissions. Measurements of emission factors of SO₂, size resolved aerosols and their chemical constituents for Indian cooking stoves are needed to refine the present estimates.     

Present and potential future contributions of sulfate,black and organic carbon aerosols from China to global air quality,premature mortality and radiative forcing

Aerosols are harmful to human health and have both direct and indirect effects on climate. China is a major contributor to global emissions of sulfur dioxide (SO₂), a sulfate (SO₄^2?) precursor, organic carbon (OC), and black carbon (BC) aerosols. Although increasingly examined, the effect of present and potential future levels of these emissions on global premature mortality and climate change has not been well quantified. Through both direct radiative effects and indirect effects on clouds, SO₄^2? and OC exert negative radiative forcing (cooling) while BC exerts positive forcing (warming). We analyze the effect of China's emissions of SO₂, SO₄^2?, OC and BC in 2000 and for three emission scenarios in 2030 on global surface aerosol concentrations, premature mortality, and radiative forcing (RF). Using global models of chemical transport (MOZART-2) and radiative transfer (GFDL RTM), and combining simulation results with gridded population data, mortality rates, and concentration–response relationships from the epidemiological literature, we estimate the contribution of Chinese aerosols to global annual premature mortality and to RF in 2000 and 2030. In 2000, we estimate these aerosols cause approximately 470 000 premature deaths in China and an additional 30 000 deaths globally. In 2030, aggressive emission controls lead to a 50% reduction in premature deaths from the 2000 level to 240 000 in China and 10 000 elsewhere, while under a high emissions scenario premature deaths increase 50% from the 2000 level to 720 000 in China and to 40 000 elsewhere. Because the negative RF from SO₄^2? and OC is larger than the positive forcing from BC, Chinese aerosols lead to global net direct RF of ?74 mW m^?2 in 2000 and between ?15 and ?97 mW m^?2 in 2030 depending on the emissions scenario. Our analysis indicates that increased effort to reduce greenhouse gases is essential to address climate change as China's anticipated reduction of aerosols will result in the loss of net negative radiative forcing.     

Using NOx and CO monitoring data to indicate fine aerosol number concentrations and emission factors in three UK conurbations

It is increasingly accepted that although exposure to elevated concentrations of PM₁₀ is associated with an increased risk of mortality and morbidity, the relationship may not be causal. Rather, there is evidence that number concentrations may be a more appropriate metric than mass concentrations in evaluating health risk. Number concentrations are not routinely monitored and spatial and temporal patterns are poorly quantified. CO and NO_x are co-pollutants with their major urban source in common with fine particles, i.e. road vehicle emissions; are routinely monitored in many cities and are also related to ill health. Datasets of particle number concentration measurements from approximately month-long field campaigns in Manchester, Edinburgh and Birmingham (UK) are compared with simultaneous concentrations of CO and NO_x from nearby fixed monitors. It was found that it might be possible to reliably predict particle number concentrations (diameters>100 nm) on an hourly basis in Manchester city centre from knowledge of NO_x or CO concentrations alone. The influences of meteorology, spatial variability in emissions and lack of co-location upon the correlations are investigated using cluster analysis. The cluster analysis revealed that these relationships may vary between cities and are dependent upon monitor location but in ways that can be ascribed. For two out of three sites there existed a linear relationship between average cluster aerosol and gas concentrations. This indicates that although airmass aging disrupts the short-term linear relationship, the relationship in the average survives. An emission ratio of particles (approx. 100–500 nm diameter) to NO_x of approximately 50 cm⁻³ ppb⁻¹ was estimated in Manchester and Birmingham. Particle mass spectrometry measurements indicated that organic compounds dominated these particles and an emission rate of 0.58 ton km⁻² a⁻¹ of organic particulate matter from road transport has been estimated for the Greater Manchester conurbation.     

Modelling NOx from lightning and its impact on global chemical fields

We have used a three-dimensional off-line chemical transport model (CTM) to assess the impact of lightning emissions in the free troposphere both on NO_x itself and on other chemical species such as O₃ and OH. We have investigated these effects using two lightning emission scenarios. In the first, lightning emissions are coupled in space and time to the convective cloud top height calculated every 6 h by the CTM's moist convection scheme. In the second, lightning emissions are calculated as a constant, monthly mean field. The model's performance against observed profiles of NO_x and O₃ in the Atlantic and Pacific ocean improves significantly when lightning emissions are included. With the inclusion of these emissions, the CTM produces a significant increase in the NO_x concentrations in the upper troposphere, where the NO_x lifetime is long, and a smaller increase in the lower free troposphere, where the surface NO_x sources dominate. These changes cause a significant increase in the O₃ production in the upper troposphere and hence higher calculated O₃ there. The model indicates that lightning emissions cause local increases of over 50 parts per 10¹² by volume (pptv) in NO_x, 200 pptv in HNO₃ and 20 parts per 10⁹ by volume (ppbv) (>40%) in O₃. In addition, a smaller increase of O₃ in the lower troposphere occurs due to an increase in the downward transport of O₃. The O₃ change is accompanied by an increase in OH which is more pronounced in the upper troposphere with a corresponding reduction in CO. The method of emission employed in the model does not appear to have a significant effect globally. In the upper troposphere (above about 300 hPa) NO_x concentrations are generally lower with monthly mean emissions, because of the de-coupling of emissions from the model's convection scheme, which vents NO_x aloft more efficiently in the coupled scheme. Below the local convective outflow altitude, NO_x concentrations are larger when using the monthly mean emissions than when coupled to the convection scheme, because the more dilute emissions, and nighttime emissions, lead to a slower NO_x destruction rate. Only minor changes are predicted in the monthly average fields of O₃ if we emit lightning as a monthly constant field. However, the method of emission becomes important when we make a direct comparison of model results with time varying data. These differences should be taken into account when a direct comparison of O₃ with measurements collected at particular times and locations is attempted.     

A revised estimate of copper emissions from road transport in UNECE-Europe and its impact on predicted copper concentrations

Comparisons of measured and model-predicted atmospheric copper concentrations show a severe underestimation of the observed concentrations by the models. This underestimation may be (partly) due to underestimated emissions of copper to air. Since the phase out of asbestos brake lining material, the composition of brake lining material has changed and may contain up to ∼15% copper. This makes brake wear from vehicles potentially an important source of atmospheric (particulate) copper concentrations. In this paper, we reassess the copper emissions due to exhaust emissions and brake wear from road transport. Overall, our reassessments result in an estimate of total copper emission to air in UNECE-Europe of 4.0–5.5 ktonnes yr⁻¹, which is substantially higher than the previous estimate of 2.8 ktonnes yr⁻¹. Copper concentrations over Europe are calculated with the LOTOS-EUROS model using the revised emission data as model input. The results show that the revised emission estimates are a major step towards gap closure of predicted versus observed copper concentrations in ambient air. Brake wear emissions may be responsible for 50–75% of the total copper emissions to air for most of Western Europe. The hypothesis that road transport is an important source of copper emissions is tested and confirmed by (1) reviewing available literature data of chemically speciated PM data from road tunnel studies and (2) the gradient observed in copper concentrations from ambient PM monitoring going from rural sites to street stations. The literature review and observational data suggest that the majority of the emitted PM10 brake wear particles is in the PM2.5–10 size range. The results of this study indicate that modification of brake lining composition is an important mitigation option to reduce copper exposure of the population in Western Europe.     

On-road remote sensing measurements and fuel-based motor vehicle emission inventory in Hangzhou,China

Motor vehicles are one of the largest sources of air pollutants worldwide. Despite their importance, motor vehicle emissions are inadequately understood and quantified, esp. in developing countries. In this study, the real-world emissions of carbon monoxide (CO), hydrocarbons (HC) and nitrogen oxide (NO) were measured using an on-road remote sensing system at five sites in Hangzhou, China in 2004 and 2005. Average emission factors of CO, HC and NO_x for petrol vehicles of different model year, technology class and vehicle type were calculated in grams of pollutant per unit of fuel use (g l⁻¹) from approximately 32,260 petrol vehicles. Because the availability of data used in traditional on-road mobile source estimation methodologies is limited in China, fuel-based approach was implemented to estimate motor vehicle emissions using fuel sales as a measure of vehicle activity, and exhaust emissions factors from remote sensing measurements. The fuel-based exhaust emission inventories were also compared with the results from the recent international vehicle emission (IVE) model. Results show that petrol vehicle fleet in Hangzhou has significantly high CO emissions, relatively high HC and low NO_x, with the average emission factors of 193.07±15.63, 9.51±2.40 and 5.53±0.48 g l⁻¹, respectively. For year 2005 petrol vehicles exhaust emissions contributed with 182,013±16,936, 9107±2255 and 5050±480 metric ton yr⁻¹ of CO, HC and NO_x, respectively. The inventories are 45.5% higher, 6.6% higher and 53.7% lower for CO, HC and NO_x, respectively, than the estimates using IVE travel-based model. In addition, a number of insights about the emission distributions and formation mechanisms have been obtained from an in-depth analysis of these results.